Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , 7 , , 5 , 1 1 , , , 6 1 1,* , 11,16 1,11 , 6 , L. V. Rizzo , N. F. da Silva 1 , I. Trebs 7 , T. Könemann , J. Williams , A. C. Nölscher 1 , C. M. de 17,19 1 1 1 , C. B. Sales , C. G. G. Barbosa 5 15 , U. Pöschl 1 , J. Tóta 7 , A. F. L. Godoi , B. Weber 1 , M. Sörgel 1 , B. B. L. Cintra 1 1,7 , J. Kesselmeier , P. Artaxo 4 10 , M. D. O. Sá , R. Ditz , and A. M. Yáñez-Serrano 1 , C. Pöhlker , D. Moran-Zuloaga 14 , X. Chi 7 , Z. Wang 5 11 1,11 1 , N. Targhetta 11599 11600 mann ff 1 ff , A. Araùjo , J. Schöngart , F. Ditas 3 1 , H. Su , T. Ho , S. Wol 8,11 , L. D. A. Sá 9 1 17 , D. Walter 1 , S. Carbone , A. O. Manzi 10 5 9 , M. T. F. Piedade , J. Saturno 12,** 17 , J. Brito 5 , O. C. Acevedo , M. Heimann , F. Wittmann 6 1,2 , J. V. Lavric , A. van Eijck 1,9 1 9 , N. Ruckteschler , C. Q. Dias-Júnior , R. A. F. de Souza 6 13 11,18 Department of Chemistry, Johannes GutenbergInstituto University, Mainz, Nacional Germany de Pesquisas da Amazônia (INPA), Clima e AmbienteCentro (CLIAMB), Gestor Av. e Operacional do Sistema de Proteção daDepartment Amazônia of (CENSIPAM), Belém, Chemistry, Inha University, IncheonCentro 402-751, Regional Korea da Amazônia, Instituto Nacional de Pesquisas EspaciaisInstituto (INPE), Nacional Belém, de Pesquisas da Amazônia (INPA), LBA, Av. AndréCentro Araújo de 2936, Estudos Superiores deUniversidade Parintins do (CESP/UEA), Estado Parintins, do Amazonas, Amazonas Brazil Universidade (UEA), Federal Manaus, do Amazonas, Amazonas Brazil (UFAM/ICSEZ-Parintins), Parintins,Universidade Amazonas, Federal Brazil do Oeste do Pará – UFOPA, Santarém, Pará, Brazil This discussion paper is/has beenand under Physics review (ACP). for Please the refer journal to Atmospheric the Chemistry corresponding final paper in ACP if available. Biogeochemistry, Multiphase Chemistry, and Air Chemistry Departments, Max Planck Scripps Institution of Oceanography, University of California San Diego, LaUniversidade Jolla, Federal CA Santa 92037, Maria, Dept.Empresa Fisica, Brasileira 97119900 de Santa Pesquisa Maria, Agropecuária RS, (EMBRAPA), Brazil Trav. Dr. Enéas Pinheiro, Instituto de Física, Universidade de São Paulo (USP), RuaDepartment do Matão, of Travessa Environmental R, Engineering, 187, Federal CEP University of Paraná UFPR,Instituto Curitiba, Nacional PR, de Pesquisas da Amazônia (INPA), MAUA group, Av. AndréInstituto Araújo Nacional 2936, de Educação, CiênciaMax e Planck Tecnologia do Institute Pará for (IFPA/Bragança), Biogeochemistry, Pará, Hans-Knöll-Straße Brazil 10, 07745 Jena, Germany now at: Luxembourg Institute of Science and Technology, Environmental Research and S. Trumbore J. Winderlich C.-U. Ro R. M. N. D. Santos Souza 1 Institute for Chemistry, P.O. Box2 3060, 55020, Mainz, Germany USA 3 4 Belém-PA, CEP 66095-100,5 Brazil 05508-900, São Paulo,6 SP, Brazil Brazil 7 Manaus-AM, CEP 69067-375,8 Brazil 9 10 11 André Araújo 2936,12 Manaus-AM, CEP 69083-000, Brazil Pará, Brazil 13 14 Pará, Brazil 15 Manaus-AM, CEP 69067-375,16 Brazil 17 18 19 * Innovation (ERIN) Department, 4422 Belvaux, Luxembourg D. Santos Nogueira M. L. Krüger The Amazon Tall Tower Observatory (ATTO) in the remote Amazonoverview Basin: of first results fromecology, ecosystem meteorology, trace gas, and aerosol measurements M. O. Andreae Atmos. Chem. Phys. Discuss., 15, 11599–11726,www.atmos-chem-phys-discuss.net/15/11599/2015/ 2015 doi:10.5194/acpd-15-11599-2015 © Author(s) 2015. CC Attribution 3.0 License. N. L. Dias R. H. M. Godoi H. M. J. Barbosa Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , 2 erent heights, complemented by a vari- ff 11602 11601 The Amazon Tall Tower Observatory (ATTO) has been set up in a pristine rain forest on leave from: Amazon Regional Center, National Institute for Space Research [INPE], ety of additional species measured during intensive campaigns (e.g., VOC, NO, NO ecological survey including aest biodiversity region assessment surrounding has the been site.2012, conducted Two 80 and in m the towers a have for- crometeorological 325 been m and operated atmospheric tower at chemical the variables is wererange site initiated nearing has since in completion continued 2012, and to in their crometeorological broaden measurements mid-2015. over include Measurements the temperature and of lastwater wind and few mi- energy profiles, years. fluxes, precipitation, turbulence The components, soilfluxes, meteorological temperature radiation profiles and and fluxes, mi- soil and heat profiles visibility. A of tree temperature, has lighttrace been intensity, gas instrumented and measurements to water comprise measure contentmonoxide, stem methane, continuous in and cryptogamic monitoring ozone covers. of The at carbon 5 dioxide, to carbon and 8 OH di reactivity). Aerosolmade above optical, the microphysical, canopy and asand absorption, well chemical aerosol as measurements fluorescence, in number are composition, the and cloud canopy volume condensation space. size nuclei They distributions, (CCN) include chemical tial concentrations, light results and from scattering hygroscopicity. Ini- ecological, meteorological,presented in and this chemical paper. studies at the ATTO site are region in the central Amazon Basin, about 150 km northeast of the city of Manaus. An Abstract The Amazon Basin playsatmospheric key chemistry, roles and in biodiversity. Ithuman the activities, already and carbon has more and pervasive been changeIt water changed is is cycles, expected significantly therefore to climate by essential occur in change, toline the establish record next long-term decades. of measurement present-day sitesthat that climatic, will provide be biogeochemical, a operated and base- overhuman atmospheric coming perturbations decades conditions increase to and in monitor the change future. in the Amazon region as ** Belém, Pará, Brazil Received: 19 March 2015 – Accepted: 29Correspondence March to: 2015 M. – O. Published: Andreae 21 ([email protected]) AprilPublished 2015 by Copernicus Publications on behalf of the European Geosciences Union. 5 15 20 25 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ± . Part of this de- 2 -driven carbon uptake com- 2 increases in the atmosphere, and 2 11604 11603 . A comprehensive analysis of the role of land 1 − partially compensated for by a carbon sink in trop- 1 − accounted for 38 % of anthropogenic CO 0.5 Pga 1 ± − , of which about 80 % is covered with rain forest (Goulding 0.5 Pga 2 ± ecting ecosystems and air quality in many parts of the Basin. ff km 6 0.5 Pga . The most recent global carbon budget estimates indicate that in the 10 ± 2 , or about 9 % of all anthropogenic carbon emissions (Le Quéré et al., × 1 − in the 1990s and early 2000s, consisting of a gross tropical deforestation 1 − orestation, regrowth, and uptake by intact vegetation, the main gross sinks. Us- ff 0.5 Pga ± The “net” land use emissions, as presented above, are always the sum of “gross” Depending on the path land use change takes and the interactions between the for- pensating the large deforestation source (Schimelcontinent, et al., a 2015). For detailed the South budgeting American study also concluded that carbon uptake by the bio- release and uptake fluxes, whereand deforestation a represents the dominant gross source, crease in the relative contribution fromin land use fossil change fuel is of emissions, courserecent but due years, to there particularly the in has increase the been Brazilian a Amazon significant (Nepstad et decrease al., in 2014). deforestation in ing an approach based onestimated forest inventories that and land tropical use0.7 land Pga budgeting, Pan use et al. changecarbon (2011) represented emission of a 2.9 net carbon sourcevegetation of in 1.3 the globaltropics carbon are cycle approximately balanced, concluded with that regrowth carbon and CO sources and sinks in the ical forest regrowth of 1.6 decade of 2004–2013 land0.9 use change worldwide resulted in a net carbon release of est biota and theatmospheric CO changing climate, the Amazon can act as a net source or sink of because of their potential to gainand or climate lose change. large A amounts recent of study carbonon shows as the a a strong tropical result correlation continents of between land and climateindicates use the change that rate the at strength which of2014). CO this The feedback interaction has between doubledthe physical since climate largest the and uncertainties 1970s the (Wang inhuman biosphere et the emissions represents al., of assessment one greenhouse of of gases. the response of the climate system to 2014). This represents a significantemissions of decrease 1.5 since the 1960s, when land-use carbon et al., 2003). It containsaboveground 90–120 biomass PgC in in living Latin(Baccini biomass, America representing et and about al., ca. 84 2012; % 40 Gloorsoils of % et – the of putting al., this all 2012). in tropical Anotherin perspective, 160 forests the the PgC Amazon Earth’s worldwide atmosphere holds are before about stored the halfmagnitude in industrial as of the revolution much (Gloor Amazon’s this carbon et as carbon al., was Amazon 2012). reservoir, forest Given it the in is particular, have clear the that potential tropical to forests play in a general, crucial role and in the climate change 1 Introduction A little over thirty yearsentitled ago, “Amazon Eneas Basin: Salati A and Systema Peter in Vose paradigm Equilibrium” published shift (Salati a has and landmark occurredtific Vose, paper 1984). in community, Since the which then, minds is ofof reflected the prominent in public Amazon the at researchers, “The large2012). title Despite Amazon as of its Basin well reassuring a in as title, recent Salati transition” theing and synthesis (Davidson scien- threats Vose’s paper et paper to had al., the by already pointedlarge-scale integrity a at of deforestation. grow- group the Deforestation Amazonto has ecosystem, abate mostly indeed resulting in continued, from recenttion and continued years. (Fraser, has It 2014), only goes a And, hand begun whereas Salati in and hand Vosenomenon were with concerned driven road with by climate construction change deforestationnow and as and is urbaniza- a its regional on phe- impact thezon on interactions forest the ecosystem of (Keller hydrological global et cycle,key al., climate roles 2009). the change In the focus with the Amazon following thesetting is sections, up playing functioning we a in will of long-term present the the measuring the global station Ama- ecosystem, for which monitoring1.1 its form functioning the and rationale health. for Carbon cycle The Amazon Basin covers about one thirdover of about the South 6.9 American continent and extends 5 5 15 20 25 10 20 25 10 15 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | to 1 − a 2 − ) in intact Ama- 1 − a 2 through the lowest few km of 2 outgassing (Richey et al., 2002; Abril et al., 11606 11605 2 fluxes from eddy covariance measurements dif- 2 ), mostly as a result of biomass burning, with no signif- 1 − a 2 , and it became clear that issues related to nighttime fluxes and − 1 − a 2 − (Steinkamp and Gruber, 2013). Gloor et al. (2012) have reviewed the 1 − ects make upscaling of CO ff 0.9 Pga orts to upscale local measurements to larger scales have also lead to inconclu- ff ± An intermediate scale between global inverse modeling and plot-size flux and in- Attempts to verify these carbon budgets with measurements have remained incon- E An alternative approach to upscaling from local to regional carbon balances is fol- Seen together, these studies suggest that the Amazon Basin teeters on a precarious numerous attempts to deduce theeling South and American came carbon to budgets themeaningful from conclusion results, inverse that mod- a they are conclusionvegetation not models that adequately for larger constrained they time to extend and produce to space scales. the application of digital global zon forests (e.g., GraceBut as et more studies al., were 1995; conducted, this Carswell range et expanded from al., a sink 2002; of de 8 tha Araújo et al., 2002). sive and often contradictorytechnique results. initially Flux suggested measurements a using fairly the large eddy carbon covariance sink (1–8 tha terrain e ficult to impossible (de Araujoflux et measurements al., are 2010, essential and for references understandingprocesses therein). micrometeorological and Nevertheless, and such for ecological monitoring changes in the functioning oflowed the in forest the ecosystem. RAINFOR project, wheredecades some for 140 standing forest biomass plots (Phillips havecarbon been et uptake monitored al., over by 2009). This intacthas study been forest, suggested proposed interrupted substantial that a bysites large is biomass fraction compensated of loss by the during rare uptake disturbance extrapolated drought from events, years. such the RAINFOR as It forest blow-downs resulting a source of 1.4 tha was extended to includeet the al., southern 2014). and The westernbiosphere results parts to from of be 2010, sensitive thetation. an to Amazon The unusually drought, Basin following dry resulting (Gatti year, in year,an 2011, show net approximately was neutral the carbon carbon wetter Amazon emission balance, than forest from withthe average, a biomass the and modest burning vege- biospheric source. the sink Basin compensating returned to balance between being a source orture sink depending of carbon on to the the extent world’s and atmosphere, form with its of fu- climate change as well as on human actions. icant net flux to or from the forest biosphere (Gatti et al., 2010). In 2010, this study ventory studies is captured bythe aircraft troposphere. soundings This of method CO of averages regional km. fluxes Early on measurements scalesChou during et of the al. tens (2002), 1987 to and ABLE-2near hundreds suggested experiment a Manaus. were near-neutral A carbon reanalyzed series balance by tion for of season their study flights also region north revealedapproximate that of balance daytime Manaus (Lloyd carbon et during uptakenear al., the Santarem and 2007). 2001 in nighttime A the wet-to-dry release eastern 10carbon year transi- Amazon were source aircraft concluded in (0.15 that profiling tha the study fetch conducted region was a small net from severe thunderstorms (Chambers etanalysis al., from 2013, the and RAINFOR references project, therein). nowcates The based latest that on the 321 Amazon plots carbon andpast sink 25 decade years in of compared intact data, to forest indi- the hasmortality, possibly declined 1990s. caused by This one-third by appears during greater toon climate the be mortality variability driven (Brienen and by et feedbacks increased al., ofalso biomass 2015). faster miss Like growth the flux-tower contributions measurements, of biomassmake wetlands inventories and a water substantial bodies to contribution2014). the to carbon flux, CO which may clusive so far. Thewhich derive largest fluxes from spatial concentration measurementsearly scale and attempt global is transport deduced models. represented An a2007), by large whereas global tropical a inversion sink1.1 models, more from inverse recent modeling analysis (Stephens suggests et a al., net tropical carbon source of sphere at present approximatelyfossil compensates fuel the burning, emissions withrecent from a period slight deforestation (Gloor trend and et in al., 2012). the continent becoming a source in the most 5 5 25 20 15 10 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ect ects ff ff O), both may lead 2 2 ) and nitrous oxide (N 4 C, and warming is expected to continue ◦ 11607 11608 vs. the fraction that is transformed to water vapor by ff ects of human actions, especially deforestation, global and ff ects of smoke aerosols from fires in Amazonia on cloud processes can a ff Evaporation of water from the Earth’s surface also supports a huge energy flux in Our ability to prognosticate the possible outcomes for the Amazon ecosystem in Ultimately, the fate of the carbon stored in the Amazon Basin will depend on the inter- sult, the hydrological cyclesupports of the life Amazon within Basin theBasin is Basin from crucial and the for Atlantic even providing Ocean beyondthrough the with its evapotranspiration water the maintains borders. that trade a Most wind flux circulation,more moisture but of important enters recirculation precipitation as the of airmasses that water move becomes2012). into increasingly the When western part reaching ofresult the the that Basin Andes, (Spracklen Amazonian et moisture evaporation al., even(Gimeno becomes supports et deflected the al., southward, rain-fed 2012). agriculturethe with As in e the a Argentina result, perturbations of the Amazonian moisture flux and 2009). Changes in landand cover, type e.g., of conversion clouds of overof the forest rain region to that (e.g., pasture, flows Heiblum alter away et as the al., runo 2014) amount and shift the proportion the form of latentancy when heat, the which water vapor isone condenses of to converted cloud the to droplets. major This sensible forces heat heat transfer that represents and drive atmospheric atmospheric buoy- circulation at all scales (Nobre et al., of which have importantD’Amelio sources et in al., the 2009; Amazon Beck et wetlands al., or 2012). soils1.2 (Miller et al., Water 2007; and energy cycle The Amazon River has20 by % far of the the greatestlargest world’s discharge river freshwater of in all discharge discharge. thethrough and the This World’s five water rivers reflects times bodies, – soils, the that about plants, immense and of amount atmosphere the of of the Congo, water Amazon the Basin. that next As is a re- cycling rainfall even over the distant2014). La Plata Basin (Camponogara et al., 2014; Zemp et al., the coming decades isprocesses in severely climate/vegetation curtailed models, byconnections including between limitations the the role in Amazon and of the the the Atlantic representation Andes and of and Pacific Oceans. the key In tele- addition, the evapo-transpiration (Silva Dias etand al., references 2002; therein). Davidson This et inpatterns, al., turn and 2012; changes local consequently Gloor and et deforestationfor regional al., has hydropower circulation generation 2013; and been in rainfall Amazonia predicted (Sticklerestation to et exceeds al., reduce some 2013). the 40 When % potential thechange of scale the the of functioning Basin, defor- of these theNobre perturbations entire and Amazon of Borma, climate the 2009). and water ecosystem cycle (Coe may et al., 2009; to more net carbon uptakeremote by sensing the can intact provide forest importantest vegetation information to (Schimel on changing et the climate al., and response 2015). ecological of While factors, the the Amazon recent for- controversy about the e regional climate change, and2006; changing Poulter atmospheric et composition (Soares-Filho al.,2014; et 2010; Nepstad al., Rammig et et al.,the al., 2014; carbon 2010; Schimel cycle Davidson et with etand the al., phosphorus cycles al., 2015; are of 2012; Zhang also other et Cirino likelyequally key to al., et biospheric to play 2015). two elements, al., important other Interactions especially roles greenhouse nitrogen of (Ciais gases, et methane al., (CH 2013). This applies acting and often opposing e The region has already(Malhi warmed and by Wright, 0.5–0.6 2004).(Saatchi Together with et the al., increased 2013), frequencywill the of be enhanced drought occurrence and episodes of theet periods likelihood al., of of 2013; destructive net understory Balch,increase biospheric fires in 2014; carbon will Amazon River Zeri emissions increase discharge (Gloor etetation may reflect (Gloor al., an et increasing 2014). al., water 2013), On supply which to the together the other with veg- increasing hand, atmospheric the CO observed 20 % of seasonal change andportant drought long-term on ground based the observationssystem “greenness” are (Soudani of to and our Francois, the 2014; understanding forest Zeri of illustrates et the al., Amazon how 2014). im- 5 5 15 25 10 20 25 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 2 ), carbon x are largely 4 ectively washed out by rain. The ff erent tree species. Scientists still do not ff 11609 11610 ) or the hydroxyl radical (OH). Production of these atmo- 3 Much of the Amazon’s aboveground biomass is in its trees, and a single hectare The functioning of this self-cleansing mechanism is challenged by human activities 1.4 Atmospheric composition and self-cleansing The tropical atmosphere hassphere” been by referred P. Crutzen to (personal asbiosphere communication, release the 2013). huge Both “washing amounts human machine of activities substances of and such the as the nitrogen atmo- oxides (NO know how many tree species16 000 occur tree in species the isdata. Amazon, the and result Surprisingly, of the a an current relatively extrapolationof estimate from small of all the number about existing individual (227 scatteredfraction census species, trees of or the (ter Amazon’s 1.4 ecosystem Steege %) services.Amazonian This account et biogeochemistry, fact for may for al., greatly example half facilitate 2013), studies researchplants in on which and the the therefore trace atmosphere. gas account exchange for between a large of the forest can be home to over 100 di and temperature remains verymeasurements poorly and understood process (Davidson studiesour et at understanding al., of key 2012). these locations interactions. Long-term are urgently needed1.3 to improve Biodiversity The Amazon Basin containstems the in most the species-rich world (Hoorn terrestrialplant et and species, al., over freshwater 2010; 400 ecosys- Wittmann mammal,brate et about and al., microbe 1300 2013). species bird, It (dathe houses and Silva at countless world’s et least species numbers 40 al., of diversity. 000 2005), Ofscientifically, inverte- and accounting these, possibly for the never about great will 10–20directly be. majority % related The of has to variety all the not of variety yet species ofexploitation been in habitats, that and the described is consequently Amazon accompanied is Basin threatened bydeforestation. is by habitat The any destruction, genetic form in of information particularsity stored land is in beyond clearing these measure and ecosystems andis may and now be their of under biodiver- enormous great economicother threat, significance. land mostly This use diversity changes as (Vieira a et result al., of 2008). habitat loss due to deforestation and monoxide (CO), and volatilemust be organic constantly compounds removed (VOC)gases again are into to poorly the prevent soluble accumulation atmosphere, inself-purification to water, which of and toxic the are levels. thus Most atmosphere nottrace therefore such e substances requires are chemical brought reactions intobegin by with water-soluble which an form. the initial These oxidation reaction stepmolecule, in chains such which normally as the trace ozone gas (O spheric is attacked detergents by a requires highly UV reactive in radiation generous and quantities water in vapor,the the both region tropics. of in It which comes which many thus are atmospheric as present trace no gases, surprise including that CO the and tropics CH are biophysical response of the vegetation to changing water supply and increasing CO ing and industrial activities. Thisducing may convert photochemical the smog “washing with machine” high intopollutants, a concentrations and reactor of large pro- ozone quantities and ofof other fine clouds atmospheric aerosols and – which precipitationet in al., and turn 2010). thus influence Increased the modifyburning ozone formation emissions, the concentrations have also water over been Amazonia, cycle implicateddecrease resulting in (Andreae, plant the from damage, carbon 2001; biomass which uptake may Pöschl by substantially the Amazon forest (Pacifico et al., 2015). that change the emissions from the biosphere and add pollutants from biomass burn- eliminated (Crutzen, 1987). Recentcycles discoveries in indicate the boundary that layer thebut are much atmospheric the more oxidant mechanisms active than of hadet these been al., reactions previously 2008; assumed, are Martinez still et al., a 2010; matter Taraborrelli of et al., active 2012; research Nölscher (Lelieveld et al., 2014). 5 5 20 25 10 15 10 25 20 15 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , and 3 ,O x 11612 11611 O, and a multitude of reactive gases, including NO ected by climate change. 2 ff , CO, N 4 , CH 2 climate conditions and anthropogenic influences. lower troposphere, within and outside the planetary boundary layer, in order to Specific objectives are: The continuous long-term data collected at ATTO will also serve to evaluate airborne For this purpose, the Amazon Tall Tower Observatory (ATTO) has been established The concentrations and types of aerosol particles over the Amazon Basin exhibit 1. To understand the carbon budget of the Amazonian2. rainTo forest continuously under observe changing anthropogenic and biogenic greenhouse gases in the unique observatory in South America willAmazonian provide ecosystem long-term a observations of the tropical and satellite observations. Expected to operate for an indeterminate length of time, this VOC, as well as a broadare range complemented of by aerosol a characteristics. full Thethe suite chemical observing of measurements system micrometeorological will measurements. also Furthermore, tion include canopy, such a as component phenological directed observationspotentially at from a the the canopy underlying tower lidar, by vegeta- as automatedbiological well cameras, variables as in an the array ecosystems of near in-situ the sensors tower and of the critical ground. physical and a basis for continuous monitoringsuch of as long-lived CO biogeochemically important trace gases in the central Amazon Basinup by a initially Brazilian-German with partnership. two Thestruction site measurement of has towers a been of 325 set mrepresenting intermediate tall large height tower footprints (80 to m), perform is and chemical currently the and nearing meteorological con- completion. measurements The tower will serve as This is true especiallyare in rapidly view changing, of and thethese that fact changes. that continuing It the observations is Amazonpresent are particularly atmospheric and essential and urgent its ecological to to conditions global keep beforethe obtain environment upcoming track eastern baseline changes, of part especially data of in now, the to Basin, document will forever the change the face of Amazonia. tem. While considerable knowledge hasclear been gained that from the campaign-style full studies,long-term it picture is will studies not are emerge required from at these key “snapshots,” but locations that (Hari continuous, et al., 2009; Zeri et al., 2014). 1.5 The Amazon Tall Tower Observatory (ATTO) The foregoing sections haveBasin thrown in some the Earth highlightsident System on that and the we the key need importantatmosphere role a ecosystem in better of services this understanding the it important of Amazon provides. region the It to interactions is avoid between ev- irreversible biosphere damage and to this complex sys- 2004). These changes in theradiation atmospheric budget, aerosol cloud burdens physics, have precipitation, strong2002; and impacts Williams plant on et photosynthesis the al., (Schafer et 2002;Freud al., Andreae et et al., al., 2008; 2004;et Lin Bevan al., et et 2014). al., al., Episodic 2006; inputs 2009; Oliveiraaerosols of Martins et transported Saharan al., dust, et over 2007; biomass al., long smokepicture 2009; from distances (Formenti Africa, Sena et with and al., et the marine 2001; al.,2011). Ansmann trade 2013; et winds This al., Cirino further 2009; complexity Ben-Ami complicate ofnisms et the al., that aerosol 2010; lead sources Baars to et is(Pöhlker the al., et one production al., important of 2012; biogenic Chen reason aerosols et why al., in 2015). the Amazonia are mecha- still enigmatic huge variations in timetant and sources, and space. especially Inaerosol in the concentrations of the absence any rainy of continentalMartin season, region pollution et the (Roberts al., from et 2010b; Amazon Pöschl al., regional has etet 2001; al., or among al., Andreae, 2010; 2009; 2013). dis- the Andreae Biogenic et lowest al., aerosols,chemically 2012; either Artaxo from emitted et biogenic directly al., organic by 2013; the(Martin vapors, Rizzo biota make et or up al., produced most 2010a). photo- At ofsouthern Amazon, the this aerosol other “clean-period” concentrations extreme, aerosol over during largepolluted regions the urban are biomass as areas burning high worldwide season as (Artaxo in in the the et most al., 2002; Eck et al., 2003; Andreae et al., 5 5 25 20 15 10 25 15 20 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ects on the atmosphere and ff C and mean annual precipitation ◦ ects of land use change on the atmosphere ff 11614 11613 erent forested ecosystems. The tower site is lo- ff help constrain inverse methods forand deriving their continental source changes and over time. sink strengths standing of atmospheric chemistrya and continuous physics assessment in the of Amazon the and e further allow and climate. to our understanding of natural and anthropogenic e climate. Measurements of isotopicanthropogenically composition and will biologically induced be fluxes. made to help distinguish idant cycle, the trace gascycle exchange of between the forest Amazonian aerosol. and atmosphere, and the life ground to estimate biosphere–atmosphere exchange rates. as well as to understandover the the extent forest. and characteristics of the roughness sublayer models, and inverse modelstrace gas for fluxes. the description of heat, moisture, aerosol, and and humidity profiles. Upwind of the site in the main wind direction (northeast to east), large areas covered The USDR consists of several di 3. To continuously measure trace gases and aerosols for improvement of our under- 4. To simultaneously measure anthropogenic and biogenic trace gases, contributing 5. To investigate key atmospheric processes, with emphasis on the atmospheric ox- 6. To determine vertical trace gas and aerosol gradients7. from theTo study tower turbulence top and to transport the processes in the atmospheric boundary layer, 8. To develop and validate dynamic vegetation models, atmospheric boundary layer 9. To evaluate satellite estimates of greenhouse gas concentrations and temperature stem of the Amazon is incities the of fetch region Santarém of and ATTO, withthe scattered Belém smaller southeast, at towns the distances and densely the of populated about states 500 of and the 900 Brazilian km, Nordeste respectively. To lie at distances by mostly undisturbed terranortheast, firme the nearest forests region extend withGuyanas over dense and hundreds human of activity of Amapá is kilometers. State, in about To the 1100 the coastal km regions away. In of the the easterly direction, the main cated approximately 12 kmland NE forests of (terra the firme)130 Uatumã ma.s.l. prevail on River, Seasonally plateaus where flooded atriver dense, channel, black-water a oxbow non-flooded (igapó) lakes, maximum and up- forest altitude theproximately dominates several of 25 smaller ma.s.l.). along tributaries approximately Interspersed of the the withforests Uatumã main these on River formations ancient (ap- river are terraces non-flooded (35–45 terra ma.s.l.),soils) firme and and campinaranas campinas (white-sand (savanna on forest), white-sand whichthe are river predominantly terraces located and between the slope to the plateaus. of 2376 mm (IBGE, 2012).from The February region to is May and characterized a by drier a season pronounced from rainy June season to October (IDESAM, 2009). 2 Site description and infrastructure 2.1 Site characteristics The ATTO site isDevelopment Reserve located (USDR) 150 in kmJune the 2009 northeast Central in of Manaus, Amazon Brazilianin (Fig. Manaus and terms 1). German in of In Scientists logistical the evaluated and aThis three scientific Uatumã workshop conservation potential criteria unit sites on Sustainable and is decided 23 under tovironment the establish and control ATTO Sustainable and in Development administration the of of USDR. Amazonasis the State Department bisected (SDS/CEUC). of The by En- USDR thetropical Uatumã humid, River with through mean annual its temperature entire of NE–SW 28 extension. The climate is 5 5 25 15 20 10 10 15 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | - S, ffi ◦ erences in meteorological conditions and ff 11615 11616 The origins of the predominant airmasses at ATTO change throughout the year, as where the road ends.SE After the a landing, 61 Porto km ATTO, is motor-boatsite reached. ride on The the on access plateau road the follows from Uatumã an the old River landing trail towards to used the the in ATTO the 1980s to extract Pau Rosa wood from the forest. This trail was re-opened in 2010 and widened to an ATV and tractor tra 2.2 Access The ATTO site101 is km northward reached to from athe junction Manaus E south on of by a Presidente following pavedRamal Figuereido, side then national da road, heading Morena AM-240, highway 70 km along towards BR-174 to Balbina, the then for Uatumã 38 km River SE to on the the small dirt community road of Porto Morena, so that aern large Hemisphere part (NH). of Airmassesa the then clean Basin, fetch arrive region including predominantlyfrom covered ATTO, from with is the the rain in Atlantic northeast forest.smoke the and During over from this meteorologically Africa fires period, North- brings in long-rangewhen episodes transport West the of ITCZ Africa. moves marine This toseason flow aerosol, the at pattern north ATTO, Saharan a shifts of dust, periodthe ATTO. abruptly This of easterly and shift at time and southeasterly marks during the fetch the whichbiomass end regions, beginning the which burning of of receive site and considerable May, the is other pollution dry entire exposed from human Basin to activities is airmasses in south from northeastern ofmeteorologically Brazil. the and In ITCZ, geographically. The and July thus transition almostmore to lies the gradual, in the beginning the northeasterly in Southern flow September Hemisphere pattern and (SH) becoming is both complete only in March. chased from the Irish company UPRIGHT (formerly INSTANT). The walk-up tower can The measurement facilitiesheight, on already the implemented, ATTO and plateauSeptember 2014, the consist and 325 is of m now tall two nearingestablished completion. tower, for towers In whose pilot 2010, of an construction measurements, ca. 81measurements, which m began followed triangular 80 is in in m mast 2011 currently was by used an for 80 m a heavy-duty wide guy-wired set walk-up tower, of pur- aerosol atmospheric composition (Andreaeshows et monthly al., trajectory frequency 2012). plotsan for This elevation 9 day is of backtrajectories 1000 illustrated arriving m. at in During ATTO at boreal Fig. winter, 3, the which ITCZ can lie as far south as 20 cable path that was usedIn during 2012/13 the the initial government yearsde of Estado of de the the Infraestrutura, development State SEINFRA, ofbetween financed of the the and Amazonia, Uatumã implemented ATTO River site. a represented and 6 the by mtrucks. ATTO wide tower the The site, dirt overall which Secretaria road distance accommodates along pickups130 and this ma.s.l. road, During Ramal the ATTO, ishas years 13.7 km, been of rising gradually the from reduced project 25 fromthe development, to delivery a the of whole-day travel large time trip and from inor heavy 2009 Manaus equipment pontoon to to is Porto a possible ATTO,tributary, fluvial 4.5 h Rio transportation from Uatumã, ride by Manaus a in ship distance by 2014. of For going ca. down 550 km the2.3 and travel Amazonas time River of Camp and 2 days. up its The base camp onfrom INPA/LBA the and workers ATTO hired plateau from(USDR). was the built Uatumã The Sustainable in camp Development Reserve 2011/12 hasa by electrical dormitory a power with team and hammocksplanned of water, by that technicians INPA and can at facilities the accommodatefor include Uatumã ecological ca. research River toilets 20 in landing, and the people. which area.camp. will Another A serve helicopter camp landing also is site as is a intended base adjacent to station this 2.4 Towers the Intertropical Convergence ZoneAmazon (ITCZ) Basin, undergoes resulting large in seasonal pronounced shifts di over the greater than 1000 km. Figure 2dominant presents land on cover in overview of northern the South population America. density and the 5 5 25 10 15 20 25 10 15 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | × H) × L × azimuth to- ◦ 200 cm (W × c and provides direct ffi 420 × elevation and 273.1 ◦ erent forested ecosystems near the tower site. 11618 11617 16mm. The voltage provided to the labs is 230 ff × 10 cm DBH (diameter at breast height) were numbered, tagged with alu- ≥ A cluster of two redundant routers manages the internet tra Data communication within each site occurs via wired LAN with data rates of up to minum plates, and, whenwere possible, collected identified for in later identification theestimated by in field. a the pantropical Fertile allometric INPA herbarium, and modeltree (Feldpausch Manaus. sterile et height, The al., vouchers 2012) and AGWB considering was wood DBH, measuring specific device gravity. We (Blume–Leiss) measured and tree determined height wood with specific a trigonometric gravity by sampling All trees with Forest plots of three hafirme each on were inventoried ancient in river thea terraces, igapó, preliminarily and the description of the campinarana, the the terra floristicground terra firme composition wood and biomass on turnover (AGWB) the as in well the plateau, as di in the above- order to provide and 135 V, and UPSs areseparately being to used to avoid stabilize power energy. Poweris fluctuations to established, the at camp it the is is measurement provided 100 planned sites. kVA generators When to at the upgrade a tall the distance tower of power 2–3 generation km to downwind of a the new tower. 3 system of 2 Measurement methods 3.1 Floristic composition and biomass characterization communication with the remote ATTO sitePhonePro) and for are safety available matters, operating satellite in phones the (Isat- INMARSAT net. 2.6 Electrical power supply Electrical power is providedsites by (lab a containers system and of towers)kVA, diesel are operating generators. supplied alternately Currently, by by the two weeklyfrom 60 scientific switching. Hz the They generators with are measuring 45 located sitespower and ca. generation to 40 800 m and avoid downwind consumption, contamination.using power Due two is parallel to transmitted cables, the via each 3mm two long 600 distance V between transformers, carry a total payload offor 900 meteorological kg, and with trace outboard gas measurements. platforms79.3 The m, on measurements are 5 at the levels. the It highest topperformed is ground level, so at currently based far. used The measurements tower within coordinates theinstruments (WGS Amazonian 84) are rain are accommodated given forest in in Tableand 1. three the The greenhouse air-conditioned measuring gas containers, lab the atbase the trace of base gas of the the lab mast, walk-up tower, each and lab the aerosol with lab inside at the dimensions of 292 wards the geostationary satellite INMARSAT 4-F3 Americas. 1000 kbps. In addition, atcommunication the camp system there allows is monitoring WLANin available and all in controlling the three 2.4 of lab GHz networkable mode. containers, The instruments as well as internet e-mailing, locally and globally. For oral and supplied by 230/135 V electrical power. 2.5 Communications Since the end oflite. The 2013, uplink the is ATTOusing site realized the has INMARSAT/BGAN by broadband been the network,492 mobile connected kbps. providing Operating satellite a to in data terminal the the bandwidthcompensation Cobham L-Band, internet of of its EXPLORER by up active signal 700 to satel- antenna attenuation50 performance m due allows height up to on to bad 20 the weather. dB walk-up The tower, antenna aligned is by mounted 43.9 at access from the internet toATTO site. the The various routers computers and areremote networkable providing server instruments additional at features access, the likeVoIP optimized telephony centralized between file data the local storage, transfer, infrastructuralbetween sites, monitoring etc. the Internal systems, data various updating communication sitesa clients, wireless on LAN the bridge, ATTOdirected-beam operating plateau antennas. in (towers, the labs, 5 camp) GHz is mode, featured realized by via access points with 5 5 25 20 10 15 15 25 10 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | O in- 2 ects of H ff ), ozone / 2 2 Converter (BLC); DMT, .). The instrument is ca- 2 2 Vm 21 − 10 = as well as surface boundary layer stability 2 11620 11619 O and CO 2 O) were carried out at 8 heights, in and above the rain forest 2 C for 72 h) and fresh volume. Additionally we used data from the ◦ was determined by the same analyzer after specific conversion O are measured by non-dispersive infrared absorption techniques 2 2 and H O fluctuations are detected by three fast response open-path CO 2 2 and H ), and water vapor (H 2 3 Measurements of Volatile Organic Compounds (VOC) were performed using a Pro- During intensive campaigns, measurements of mixing ratios of Volatile Organic Com- The NO mixing ratio was determined by a gas-phase chemiluminescence technique Alteddy (version 3.9) basedsoftware on is available Aubinet in et themeans al. internet and). (www.climatexchange.nl/projects/alteddy/ (2000). Fluxes, variances Detailed were information2008, calculated about 2010). for half-hourly this intervals (de Araújo et al.,3.4 2002, Vertical profiles of reactive traceOzone gases is and measured by total a OH UV-absorption reactivity (Thermo technique with Scientific, a Franklin, Thermo MA, Scientific 49i USA), analyzer using Nafion dryers to minimize the e changing water vapor concentrations, as suggestedratios by of Wilson CO and Birks (2006). Mixing ton Transfer Reaction Mass Spectrometerstandard (PTR-MS, conditions Ionicon, (2.2 hPa, Austria) 600 operated V, under 127 Td; 1 Td cores from the treewood trunk samples and at calculating 105 theGlobal ratio between Wood dry Density mass Databasedetermined (after DRYAD (Chave drying wood et the specific al., gravityfor 2009) in tree for the species tree terra in the species firme campina without forests and and igapó from forests. 3.2 Targhetta (2012) Meteorology The walk-up tower is equippeding with a vertical suite profiles, of for standardrecorded: details meteorological sensors see (a) (includ- Table soil 2). Thetion), heat following (b) flux, quantities incoming are soil and continuously radiation moisture outgoing (PAR), short and net and soil radiation, longtemperature, ultraviolet temperature wave atmospheric radiation, (10 radiation, pressure, min rainfall, photosynthetic wind time relative active Data speed humidity acquisition resolu- and is (RH), direction realized (1 air minScientific by Inc., time several USA). resolution). data Visibility loggers is measuredGmbH, (CR3000 with and Königsmoor, an Germany), CR1000, optical fog Campbell which sensora (OFS, 650 detects Eigenbrodt nm the laser. backscattered light intensity3.3 from Turbulence and flux measurements Turbulent exchange fluxes of H are measured within and aboveThe the canopy method using is the eddy well2012) covariance documented and (EC) will in technique. not the be described literaturetions here. were (e.g., Three-dimensional measured wind by Baldocchi, and sonic 2003; temperature anemometersCO fluctua- at Foken 81.0, et 46.0 and al., 1.0 ma.g.l. (see Table 2). Boulder/USA). (Licor-7000, LI-COR, Lincoln, USA). pounds (VOC), total OH reactivity, nitric oxide (NO), nitrogen dioxide (NO frared gas analyzers installed atThe a high-frequency lateral signals distance of aredata about recorded 10 are at cm from processed 10 Hz the applying by sonic state-of-the-art path. CR1000 data correction loggers. methods The using raw the software (O to NO by a photolytic converter (Solid-state Photolytic NO (NO Chemiluminescence analyzer, model CLD TR-780,mixing Ecophysics, Switzerland). ratio The of NO canopy, using a reactive traceet gas al. profile (2007). system The similar lowerfloor) to part was that of described set the by up verticalThe Rummel at upper profile an part (0.05, 0.5, of undisturbed andmounted the location 4 vertical on m near profile the above the (12, the north-west walk-uplines 24, forest corner tower 38, (PTFE) of 53, (distance were the and fed 12 m). walk-upcontainer 79 to m 10 tower. the m above Heated analyzers, west forest and of floor) which the insulated was were walk-up intake housed tower. in the air conditioned lab 5 5 10 15 20 25 10 25 15 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , 2 1 2 O − 2 /H 4 for CO CH 1 − / 2 ) 4 cient) present in the ffi , and CH 2 , respectively. Although both CO measurements were es- 2 nities higher than water and / 4 ffi CO / CH / ] followed by 130 mg of Carbograph 2 10 Hz and is primarily used for eddy 1 − reaction rate coe ≥ g × 2 and CO 4 and CO, respectively. Both analyzers agree are used to charge the compound of interest 2 + CH 11621 11622 / O 2 3 ; the drift is quite large with 1 ppm and 3 ppbday -Axis Integrated Cavity Output Spectroscopy (OA- 4 ff for CO 1 and 7 ppb for CO. The long-term drift of the analyzer O concentration in air, these measurements are not cal- − 2 2 , the long-term drift is below 2 ppm and 1 ppbyear 4 erence below 0.02 ppm. When the G1301 analyzer broke down in and 2 ppb for CH ff 2 di 2 instruments. ]; Lara s.r.l., Rome, Italy) (Kesselmeier et al., 2002) and analyzed by GC- 1 2 − g , respectively. For the G1302, tests with a stable gas tank show a SD of the 2 4 and 0.5 ppb for CH 2 , and CO The G1301 analyzer provides data with a SD of the raw data below 0.05 ppm for In addition to the measurement of individual reactive inorganic trace gases and the Calibration was performed using a gravimetrically prepared multicomponent stan- 3 was regularly tested for linearityuide). VOC of and response total using OH antwo reactivity separate isoprene measurements PTR-MS were gas systems performed standard measuring simultaneously (Airbe with from Liq- directly the compared same over inlet, time, so height, that and the season. results may 3.5 Vertical profiles of long-lived trace gases (CO, CO In March 2012, continuous andtablished high in precision an CO air-conditioned containersample at air the inlets foot are of installedinlet the at tubes 80 five m levels: are tall 79, walk-up 53, constantlywall tower. 38, interaction flushed The 24, within at and the 4 a mhigh tubing. above flow A flow ground. rate portion lines The of of atring-down the several a spectroscopy sample liters technique. lower air The per flow is G1301Inc., rate minute sub-sampled USA) and for to are from G1302 used analysis the avoid Picarro for with measuring analyzers CO (Picarro instruments based on the cavity covariance and chamber flux measurementshighly where precise a and low stable drift long-term measurements. rateof The 0.6 is ppm FGGA less for operates vital CO with than a for raw SD pable of continuously monitoring VOCs with proton a analyzers also measure the H CO at low mixing ratiostransfer reaction (several is ppt a withcompounds soft a chemical is time ionization low. resolution More technique,1998). meaning of detailed Protonated that information about water fractionation molecules is 1–20 H s). of provided The elsewhere proton (Lindinger et al., atmosphere. Comparison of theOH directly reactivity measured of total the OHor individually reactivity unmeasured” detected to species OH the allows reactivity.ducted summed quantification Direct by of measurements the the Comparative of “missing Reactivity totala Method OH detector. (Sinha The reactivity et al., were PTR-MSing 2008) con- monitored using and the a reaction PTR-MS mixing in as and ratio a then of with Teflon-coated a glass OHcompounds. reagent reactor. in The (pyrrole) Pyrrole the after competitive presence first mix- reactionsmolecules of reacts cause of ambient with a air the change OH in containing reagentatmospheric alone the many total detected and OH levels more the of reactivity OH pyrrole. provided ambient Thisate the reactive can instrument OH corrections be is are reactive equated well applied to calibrated the and (Nölscher appropri- et al., 2012). The total OH reactivity instrument ibrated and can therefore be regarded only as informative. and CH raw data of 0.04 ppm for CO ICOS; Los Gatos Research Inc.,analyzer USA) is as designed an emergency for solution. measuring This at CO rates of prior to separation and detection bymass a to quadrupole mass charge spectrometer ratio. accordingtotal) One to their can entire VOC be vertical determined profile every (from 16 min 0.05 using to the 80 m, same 8 inlet heights system in as the NO, NO is below 2 ppm andwell 4 with ppbyear a CO VOCs, the total OHrate reactivity of was all OH-reactive monitored. molecules Total (mixing OH ratio reactivity is the summed loss 2012, it was replaced fromGas December Analyzer 2012 (FGGA) until based October on 2013 O by a Fast Greenhouse O dard (Ionimed, Apel&Riemer).packed tubes Occasionally, (130 mg samples of Carbograph were 1 collected [90 m inFID in absorbent ordermonoterpene to speciation cross-validate for the the total measurements OH by reactivity measurement. PTR-MS and to determine the 5 [560 m 5 5 10 25 20 25 15 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 2 cient ffi , and trans- ff for 450, 550, 1 − was used to convert the 1 − g 2 usion dryer, developed by the Institute ff ) of 6.6 m ). For the Aethalometer, an empirical cor- e abs α 11624 11623 cients are 0.45, 0.17, and 0.26 Mm ffi ciency ( ffi ects and absorption enhancement due to reflections from 670 nm) and a 7-wavelength Aethalometer (until Jan- ff usion driers. Since January 2015, the aerosol sample air ff = λ 370, 470, 520, 590, 615, 660, 880, and 950 nm) are used for measur- , respectively. For the time when the FGGA was used, the calibration 4 = λ and CH 2 A Multi-Angle Absorption Photometer (MAAP, Carusso/Model 5012 MAAP, Thermo For measuring aerosol light scattering, we use a three-wavelength integrating neph- Biological material is measured with the Wideband Integrated Bioaerosol Spectrom- Electron Group, USA, of aerosol collected oninclude a multiple scattering filter e is determined by radiative transfer calculations, which rection method described byscattering Rizzo artifact. et al. (2011) was used toeter correct (WIBS-4, the DMT). The data WIBS for utilizesbiological light-induced the materials fluorescence technology in to real-time detect based on the presence of fluorophores in the ambient uary 2015 model AE-31,ley, since CA, then USA, model AE33)ing (Magee the Scientific light Company, absorption Berke- byat particles. ATTO The since MAAP March and 2012. aethalometer In have the been MAAP deployed instrument, the optical absorption coe the filter. A mass absorption e as the high span gasevery and twelve air hours as using the filtered low ambient span3563 air. gas. Noise have The level been and zero investigated detection signals by limits areand/or Anderson for measured the et short once TSI al. sampling (1996).ties. At times, low For random particle the noise concentrations 300 snoise dominates ratio averages the of applied 2, nephelometer here, forand the uncertain- scattering 700 detection coe nm, limits, respectively. Since definednumber sub-micrometer as size particles distribution a at predominate signal oursuper-micron in to remote correction the continental or particle site, an thederson average sub-micron and of (as Ogren opposed the (1998) to two) weresuggested corrections that used given this for correction in the is Table truncationparticles, accurate 4 corrections. to but of within that Bond An- 2 the et % error al. for could a (2009) be wide range as of high atmospheric as 5 % for highly absorbing particles. MAAP absorption data to equivalent BC (BC after February 2014: Ecotechderson Aurora et 3000, al., wavelengths 1996; 450, Anderson 525, and and Ogren, 635 1998). nm) Calibration (An- is carried out using CO ported in aconditioned laminar container flow (aerosol lab through atbelow mast, a see 40 2.5 % Sect. cm 2.4). using diameter Thehas silica sample stainless been humidity di is dried steel kept using tube a into fully automatic an silica air- di elometer (until February 2014: TSI model 3563, wavelengths 450, 550, and 700 nm; for CO and drift correction routines werewhole adopted measurement accordingly. system, The detailed includingtines description will measurement, of be calibration the presented and elsewhere. correction rou- 3.6 Aerosol measurements 3.6.1 Size distributions and optical measurements Aerosols are sampled above the canopy at 60 m height, without size cut-o for Tropospheric Research, Leipzig, Germany (Tuchtions et are al., currently 2009). Aerosol measured size fromning distribu- 10 nm Mobility up Particle to Sizer 1010–430 µm nm), (SMPS, using TSI an three instruments: model Ultra-High a 3080,CO, Sensitivity Scan- St. USA; Aerosol Paul, Spectrometer size MN, (UHSAS, range:3330; USA; DMT, 60–1000 size Boulder, nm), size range: range: and 0.3–10 µm). anwhereas The the SMPS Optical UHSAS provides Particle and an Sizer OPS electromobilitydistributions measure size (OPS, from aerosol distribution, TSI the light particle model scatteringcontinuous scattering and above-canopy size estimate intensity measurements, the aerosol (Cai size sizewith et distributions the al., are Wide measured 2008). Range In AerosolGermany; addition Spectrometer size to range: (WRAS, the 6 Grimm nm–32 µm) Aerosolheight. from Technik, The Ainring, a WRAS separate provides inlet350 nm line electromobility below and size the uses distributions canopy particlethe at in instrumentation light 3 the setup m scattering are size for given range in the of Table size 2. 6– range above 300 nm. Details of 5 5 25 15 20 10 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | poly- ® ine tech- ffl ciency spec- ffi ). + 3 ciency (CE) of 1.0 is ffi and Fe + 2 ) are activated and form water presc S 4 h. The measurement period already ∼ ciently samples aerosol particles through ffi C). Subsequently, the evaporated gas phase 11626 11625 ◦ 2 excitation (280 and 370 nm)-emission (310–400 × erential mobility analyzer (DMA, Grimm Aerosol Technik, Ain- ff for 30 min of signal averaging. Mass calibration of the system 3 − 0.2 µgm erent supersaturation levels takes ff < sampling was carried out from 7 March to 21 April 2012 on Nuclepore 2.5 Size-resolved cloud condensation nuclei (CCN) measurements are performed us- Aerosol samples for Scanning Electron Microscopy with Electron Probe Micro- PM ing a continuous-flowcially streamwise available thermal from gradient DropletBoulder, Measurement CCN CO, Technologies, USA), counter Inc. a (model (CCNC), di CCN-100, commer- DMT, droplets. The completion of atra full at measurement 10 cycle di comprising CCN e ring, Germany) and a condensationTechnik). particle By counter (CPC changing model the 5412,set Grimm temperature Aerosol to gradient, values the between supersaturationor 0.1 of and smaller the 1.1 than %. CCNC Particles the is with prescribed a supersaturation critical ( supersaturation equal to covers 12 months and is beingmation continued. The on long-term the data size set provides dependentout unique hygroscopicity infor- the of seasons. Amazonian aerosol Thecampaigns particles (e.g., results Gunthe through- will et al., complement 2009; and Rose et extend al.,3.6.3 the 2011; Levin results et Microspectroscopic from al., analysis 2014). previous of single aerosolComplementary particles to the online long-term aerosol measurements, modern o niques were applied tocrospectroscopic aerosol techniques, samples such collected asNear-Edge at Scanning X-ray the Absorption Transmission ATTO X-ray site. Fine MicroscopyElectron Structure In Microscopy with Analysis particular, with (STXM-NEXAFS) mi- Energy and Dispersivelized X-ray Scanning spectroscopy to (SEM-EDX), shed were light uti- onnanometer resolution. the morphology and composition of single aerosolanalysis particles (EPMA) with were collected at theFor ATTO the site on collection top of of size-segregated the samples 80 m for tower single in particle April 2012. (i.e., EPMA) analysis, the capillary column CS12Ametals, was a used, CS5A for column anions, (calibrated an to AS19 quantify column, traces and of for Fe transition and 420–650 nm) matrixfactor. is recorded along with the3.6.2 particle optical Chemical size measurements and and hygroscopicity shape The submicron non-refractoryChemical Speciation aerosol Monitor (ACSM, Aerodyne, composition USA)The as is described instrument by is Ng measured a et compact al. usingtrometer (2011). version (Jayne of an et the widely al., Aerosol used 2000).an Aerodyne The aerodynamic Aerosol ACSM Mass lens e Spec- inchemical the composition 75–650 nm oftransmitted size the into range non-refractory a and species.izes detection characterizes on The the chamber a mass where focused hotcompounds and the particle surface are non-refractory beam (typically ionized fraction by at is a 70 flash 600 eV quadrupole vapor- electron mass impact spectrometer.volution and The of their chemical the spectra speciation mass determinedparticulate is spectra using organics, determined according sulfate, to via nitrate, ammonium, Allan decon- tion and et limits chloride al. are (2004). obtained withis Mass performed detec- concentrations using of size-selected ammoniumlowing nitrate the and procedure ammonium described sulfate by aerosol Ng fol- et al. (2011). A collection e particles (Kaye et al., 2005). A 2 applied (similar to Chen et al., 2015), yielding good agreementcarbonate with filters other at instruments. 80 m oncollected the over walk-up 48 tower h using periods. acence Harvard They (EDXRF) Impactor; were (PANanytical, MiniPal4) samples at analyzed were 1 by mAand Energy-Dispersive and 9 0.3 X-ray kV mA, Fluores- for 30 low-Z kV, (Nadetermined to and Cl) by internal elements, Ion Al filter Chromatographyfor cations for (Dionex, and the ICS-5000) anions other using and elements. UV-VIS conductivity Soluble for detection soluble species transition were metals. For cation separation, 5 5 10 15 20 25 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | . 1 − are not ff usive depo- and a corre- ff ) was sampled 20 min), which 1 − ∼ 2.5 99.9 %; Sigma Aldrich) s at 4, 2, 1 and 0.5 µm. ff ≥ 80–350. 99.9 %; Sigma Aldrich) mixture (8 : 2). ≥ m/z 11628 11627 , membrane width 500 µm, membrane thickness 3 erent cluster of similar particle types. N ff 4 on TFE coated borosilicate glass fiber filters (PALLFLEX, of about 500 nm. Particles below this nominal cut-o 1 − ff h 2.1mm, 1.9 µm particle size, 175 Å pore size; Thermo Scientific) 3 × The separation and analysis was performed with an UHPLC-system (Dionex Ulti- The extraction of the filters was performed with acetonitrile ( Aerosol samples for x-ray microspectroscopy were collected using a homemade sin- STXM-NEXAFS is a synchrotron-based technique and measurements were The SEM/EDX analysis was carried out using a Jeol JSM-6390 SEM equipped with in a sonicationa bath gentle nitrogen at flow at roomScientific), room and temperature. temperature the in The residue an was evaporation filter re-dissolvedsystem, unit in Millipore, (Reacti extracts 100 Bedford, Vap µL 1; were USA)/acetonitrile HPLC Fisher grade ( evaporated water (Milli-Q with water Mate 3000 series, autotive sampler, electrospray gradient ionization Orbitrap pump mass and spectrometerGold degasser) (Thermo column Scientific). coupled (50mm A to Hypersil a Q Exac- was used. The eluentsford, were USA) HPLC with grade 0.01 water %2 (Milli-Q formic % acid water HPLC and system, grade water 2 Millipore, % (eluent Bed- acetonitrile B). The (eluent flow A) rate and of acetonitrile the with mobile phase was 0.5 mLmin at a flow rateT60A20, of Pall 2.3 Life m Science, USA).pling the The filters sampling were times stored were at 6, 255 K 12, until or extraction. 24 h. After sam- 3.6.4 Chemical composition of secondary organicFilter aerosol sampling for Secondarywalk-up Organic tower at Aerosol a (SOA) height of analysis 42 m was above performed ground level. on Fine aerosol the (PM The column was held atwas a operated constant with temperature an ofAU), auxiliary 298 K a gas in sheath flow the rate gas columnvoltage of flow oven. of 15 The rate 3000 (instrument V. MS of The specific70 30 MS arbitrary 000, was AU, and units, operated a the in measured capillary the mass temperature negative range ion was of mode, 623 K, the resolution and was a spray gle stage impactor, which was operated atdeposited a quantitatively; flow however, a rate certain of fraction is 1–1.5 Lmin still collected via di The particles were collected on TEM grids covered with a thin carbon film (15–25 nm). sition and therefore available foronto the silicon STXM nitride analysis. substrates100 Aerosol nm, (Si particles Silson were Ltd., collected Northhampton,ensures an UK) appropriately for thin particle short coverageysis. sampling on Detailed the periods information substrate for ( can single be particle found anal- in Pöhlker et al.made (2012, 2014). at theElektronenspeicherring-Gesellschaft Advanced für Synchrotronstrahlung Light (BESSYZentrum Source II, Berlin (ALS, Helmholtz- für Materialien Berkeley,of und CA, the Energie instrumentation USA) (HZB), can2010). and Germany). be In A the found the detailed elsewhere soft Berliner high description (Kilcoyne spectroscopic X-ray sensitivity et regime, for al., STXM-NEXAFS thegen 2003; (O) light is as elements Follath a well carbon as et powerful (C), aS, al., microscopic nitrogen variety Na). of The (N), tool other technique and atmospherically with allows oxy- relevantchemical analyzing elements composition the (e.g., of microstructure, K, individual mixing Ca, aerosol Fe, state, particles. as well as the an Oxford Link SATW ultrathin windowitative EDX detector. calculations For EPMA, of quantitative and theCarlo qual- particle simulations and composition hierarchical wererelative cluster concentrations performed analysis for (Ro using each et di iterative al., Monte 2003) to obtain average we used a Battelle impactor with aerodynamic diameter cut-o sponding 50 % size cut-o 5 5 10 15 20 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ± in the campina/campinarana, erent canopy heights at 10 min ff 1 − ine and online aerosol measurements 0.01). ffl 26 Mgha p < ± 11629 11630 0.61; = 2 r erent forest types (2–54 %). Accordingly, the species ff 12; = n on the ancient fluvial terrace, reaching maximum values of 170 10 cm DBH were recorded in the 12 inventoried 1 ha plots, which 1 − ≥ in the igapó forest to 79 1 − in the terra firme forests. Tree species richness correlated significantly with 13 Mgha 1 − ± biomass 12 Mgha ± Starting in September 2014, we have conducted long-term measurements to moni- The floristic data indicate that the rain forests at the ATTO site combine high alpha diversity with high beta diversityregate at mainly a due small to geographicter contrasting scale, Steege local where et edaphic tree conditions al., speciesably (e.g., 2013; seg- between Tuomisto Wittmann et habitats, et and al., al., show 2003; high 2013). low values Biomass upon values well-drained upon and upland flooded C-stocksAmazonian soils, regions and vary as (e.g., nutrient-poor consider- previously Chave soils et reported al., and elsewhere 2005; for Malhi other et al., 2006; Schöngart et al., 2010). 13 Mgha carbon stocks in AGWB ( tor the activity patterns of cryptogamic covers at four di 4.1.2 Cryptogamic covers We investigate the potential ofparticles cryptogamic and covers to chemical servecommunities compounds. as of Cryptogamic a cyanobacteria, source covers algae, ofwhich lichens, comprise bioaerosol may and also photoautotrophic bryophytes host fungi, infeature other varying bacteria of proportions, and all archaea (Elbert thesemoisture et status organism follows al., the groups 2012). external A water isdry common conditions. their Thus conditions, the being poikilohydric organisms reactivated dry nature, again out meaning upon under rain, that fog, their or condensation. intervals, in which we measureties temperature directly and on water top contentof of within and biocrusts cryptogamic light growing covers intensi- on upontion the dewfall with trunk will patterns of of be a particleanalyzed of tree. release. for The particular In activation their on-site interest patterns measurements release toinvestigated cryptogamic of and check covers biogenic compared are for with aerosols correla- results (e.g., from spores). o These particles will be at the ATTO site. 4.2 Meteorological conditions and fluxes An overview of theby climatic Nobre characteristics et al. of (2009). the Thein meteorological Amazon Sect. setting Basin 2.1, of has the and ATTOity, site been the radiation, has presented basic been etc.) meteorological described at measurementsconditions the (wind, influenced site temperature, by reflect humid- local the topographypresent regional and overviews climate vegetation. of In and meteorological the theresults observations following micrometeorological that of sections characterize we micrometeorological the investigationsexchange site at of and ATTO. trace initial Since gases the and quantification aerosols of between the the rain forest and the atmosphere is and 101 included 60 families, 206 generain and the 417 terra species. firme Treeterrace, forest species the on richness campinarana, and the was the plateau, highest seasonally(Bray–Curtis flooded followed igapó by index) (Table 3). the Floristic within terra similarity plots firmewas forest highly of on variable the the between sameturnover fluvial di forest across types the rangedinundated investigated forest from plots forest were 45–65 types compared %, tovaried but was their non-flooded considerably high, counterparts between (Fig. the especially 4). studiedheights, AGWB when forest DBH ecosystems seasonally and as basal a74 result area of (Table varying 3). tree Carbon stocks in the AGWB increased from In total, 7293 trees 4 Results and discussion 4.1 Ecological studies 4.1.1 Tree species richness, composition, turnover, and aboveground wood 5 5 15 10 20 25 20 25 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | C in the dry ◦ 50 km distance) and ∼ er substantially from the ff 11632 11631 C during both seasons, whereas daytime maxima . The influence of river and/or lake breeze systems ◦ 1 − 12 km distance) or Lake Balbina ( ∼ C in March. ◦ C during the wet season and may reach slightly above 30 C, whereas the lowest temperatures prevail in the rainy season, with ◦ ◦ Rainfall in the Manaus region shows a pronounced seasonal variation, reaching the Overall, however, the precipitation patterns at the ATTO site are in good agreement Vertical profiles of temperature show clear diurnal cycles driven by radiative heating season. highest amounts in March (335.4 mm)an and annual the total lowest of amounts 2307.4 mm in atperiod August the (47.3 INMET 1961 mm), station for in to Manausseasonal for 1990 the). cycle standard (www.inmet.gov.br reference Precipitation with maximum atand values the September around (Fig. ATTO March siteespecially 7). and in follows The the minimum this interannual transition values todata variability in the from appears rainy the August season, years to 1981 athe be to fact 2010 that large high at has the deviations all also Manaus been fromApril, year, station evident but (Fernandes, the when in 2014). the regional the Therefore, ATTO mean values during from October the to years January 2012–2014 di and also in long term mean of Manaus, are likely the resultwith of its interannual variability. position in theare Central the Amazon, wettest where the ones.acts months In between as this February a period, and strong May the the driver interaction ITCZ in of reaches convective trade cloud itsITCZ winds formation southernmost and also at position sea takes the breeze and part equatorialregenerate at in during the trough. northeast their Due the westerly Brazilian to formationamounts propagation. coastline, of of the In precipitation. instability this After lines this way, theyaccompanying period, that account the the enter ITCZ for movement shifts the substantial of to thecipitation continent the zenith at Northern and position the Hemisphere, ATTO of site, thewhen with sun. the precipitation This driest is leads months formed to being mostly between less July by pre- and local September, convection. In the following months, the are around 28 during the night (Fig. 6). Therefore,at both temperature the minima and canopy maxima top arecan observed during be both seasons. observed Awarm at second air the temperature from forest minimum above the floorat during canopy the night during is canopy transported the top into dry are the around and forest. 22.5 Minimum wet temperatures season. During the day a key objective ofatmospheric the boundary ATTO layer program, is a the central study focus of here. 4.2.1 the structure and Wind behavior speed of and direction the aboveThe the wind forest canopy roses forDecember–14 June) the (based dry on half-hourly seasonsured averages at of (15 81 wind ma.g.l. June–30 speed for and November) thethe direction period and dominance mea- from the 18 of October easterly wet 2012the to trade season major 23 wind (1 July wind 2014; flows direction Fig. atare towards 5) ENE the indicate mainly is from measurement observed the site. east duringthe A during the inter-annual slight the wet north–south shift dry season, migration of which while season. of also flows This the governs seasonality the Intertropical amount can Convergence ofwind be rainfall Zone roses explained (see between (ITCZ), by Poveda daytime et and al., nighttime 2006).served was The at insignificant. variation the of Maximal site the wind are speeds about ob- 9 ms caused by the Rio Uatumãother ( thermally driven mesoscalethe circulations is sampled of air minor massesextending importance. several mainly This hundred have shows kilometers that their to the origin east within of the the4.2.2 site. fetch of the Temperature, precipitation, green and ocean radiation As is typical forstrong the central variations Amazon at Basin,throughout the the seasonal mean year timescales air (Nobrehighest temperature due et temperatures does are al., to not observed 2009). show mean during the Climatologically the of in dry high 27.5 season, the incident with Manaus a region, solar September the monthly radiation a monthly mean of 25.9 of the canopy during the day and radiative cooling of the canopy and the forest floor 5 5 10 15 20 25 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ) is 3, ζ (3) (1) ( / ζ a 0 con- , and h φ 2 q 2 erence ff = 0 represents ) and d ect of cloud is the height is the SD of a ζ ff ∗ ( a z w σ φ (RSL). It is usually is the friction velocity, roughness sublayer ∗ u flux is negative (directed downwards). In is always positive. The scalar 2 ∗ a 11633 11634 is the height of measurement and z (where ∗ (measured by the sonic anemometer), specific humidity z/z v θ . c is its turbulent scale (see Eqs. 3 and 4 below). In Eqs. (1) and (2), ∗ . (4) a ∗ a , (2) ∗ is the SD of the vertical velocity, ∗ w 2 ∗ ∗ a u u σ a u σ w ≡ σ ≡ ≡

) mixing ratio 40m. 0 ≡ − ) ζ 0 a ζ 2 ( (Williams et al., 2007). The roughness sublayer is considered to be a part of the 0 = ( The analysis is made in terms of the dimensionless SD functions Similar figures were drawn for specific times of day, namely 07:00–09:00, 09:00– In this section, we briefly show strong evidence that a simple adjustment factor that The radiation balance at ATTO as well as the albedo presents a clear di We analyzed measurements collected during April 2012 at the 39.5 m level, which is w w a 0 0 0 w right at the height of the tree tops, in terms of the turbulent scales h the Obukhov length with a zero-plane displacement height calculated as virtual temperature a scalar, and and We only analyzedcases measurements where the under sensibleis unstable heat positive flux conditions, (directed is and upwards) positive(4), (directed and considered the upwards), the absolute only the CO value latent is heat used, flux so that CO u and φ where φ 11:00, 11:00–13:00, 13:00–15:00 and 15:00–17:00 LT, in an attempt to identify periods of the RSL), as employedmethod” by dimensionless Mölder variables et al. (1999), is not able to collapse the “variance defined above. Overall resultscentration for are vertical shown velocity, virtual infunctions temperature, Figs. found in and 8–10. the CO The literature solid(see, for the for lines surface example, in layer Dias well et the above al., the figures 2009). roughness give sublayer representative 4.2.3 Roughness sublayer measurements The measurement of turbulentthese fluxes measurements over are made tall in forest the canopies so-called very often implies that depends on the factor gap modulation that intensifiesscattering. the radiation received at the surface by reflection and assumed that the RSLh extends to 2 or 3surface sublayer times of the the atmospheric height boundary ofelements layer, for the but Monin it roughness is Obukhov obstacles, too Similarityparameterization close Theory of to (MOST) the the to roughness RSL hold. hasthe Some been traditional progress made similarity in in functions the terms1999, of of and the applying references surface correction therein). layer factorsunknown. However, (see to the for universality example, of Mölder such et procedures al., remains amount of precipitation increases again,band which in coincides a with NW/SE direction theAtlantic that formation Convergence is of linked Zone a to cloud (SACZ) convectionSantos (Figueroa in and the Buchmann, and Amazon 2010). Nobre, due to 1990; the Rocha South et al.,between the 2009; wet andtion the exceeds dry the seasons. top SomeThey of episodes atmosphere were when radiation more the have frequent incident been solar during observed radia- the for wet the season, ATTO data. probably due to the e 5 5 15 10 25 20 10 15 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | . 2 (6) CO erence ff but not for , for reasons that 2 is the gradient of its a ∆ ective and vigorous coupling ff ect any chemical species, and ff , so instead we use in the air, and a a ∆ 11636 11635 ) and its reference value for the surface layer, as ζ ( a φ usivity of scalar ff presents even greater challenges for our proper understanding 2 , (5) ) ) 0 0 d d − − a a z z σ ( ( ∆ a a

ν 0 0 ν a a is the molecular di 0 0 a atmosphere w w ν

= = Nocturnal decoupling occurs rather frequently at the ATTO site, usually punctuated Finally, we tried to apply some concepts recently developed by Cancelli et al. (2012) In our case, there is no easy way to obtain Ultimately, the lack of conformity to Monin–Obukhov Similarity Theory found in these a a During daytime, intense turbulent activity provides an e between the observed value of other forests) implies that scalarmodels, which fluxes over use the MOST, are Amazontation, bound forest such to derived as have from grass larger standard ortherefore errors crops. here the We than implications can over expect for lowerthe this ATTO vege- 325 to are m a tall quite tower wide-ranging. ison instrumented On the and extent the operational, of other a theover much hand, roughness the better sublayer once forest. picture and will the emerge best strategies to model4.2.4 scalar fluxes Nighttime vertical coupling mechanisms between the canopy and the Amazon forest (Fitzjarrald and Moore,coupled, 1990; intermittent Ramos night, the et horizontal al., windhighly 2004). components variable During are temporally, weak a often in typical switching magnitude de- signs and in an unpredictable manner (Fig. 12). by intermittent mixing episodes, in agreement with previous studies made over the As a measure of the applicability of MOST, we useused the by absolute Dias value et of the al.shown di (2009), in and Fig. shown by 11.closer the A to solid relatively that lines expected stronger in by Figs. forcing 8–10. MOST is The for clearly results both are related temperature to and humidity, a behavior that is between the canopy layer and the atmospherefiles above of it. chemical As species a consequence, do vertical notof pro- commonly intense show vertical abrupt flux variations inducedthe divergence. by atmosphere Accordingly, episodes scalar are relatively fluxes well-behaved between duringthe the daytime, vertical so canopy profiles that and of their mean inferencelationships. quantities from At can night, be on achieved the usingthe other established canopy similarity hand, to re- the decouple reduced from2009; turbulence the van intensity air Gorsel often above it causes etfluxes (Fitzjarrald al., converge and to 2011; Moore, shallow 1990; Oliveira layers Bettsshort et in et time al., which al., periods. 2013). the Furthermore, In scalarsperiodicity intermittent may these turbulent provide accumulate circumstances, events episodic intensely of vertical over connection variablesome intensity cases, between and such the events canopy maya comprise and given almost night. the the atmosphere. entirety of In the scalar fluxes during to relate theet applicability al. (2012) of found that MOST theflux applicability number”, to of MOST the can be strength well predicted of by their the “surface surface forcing.Sf Cancelli where investigations (a fact that has been generally observed in the roughness sublayer over are not clear. Because noanalyses conclusive here. explanation can be found, we do not show these mean concentration between the surface and the measurement height. This suggests that CO of its turbulent transport in the roughness sublayer over the Amazon Forest. of the day whena constant better vertical agreement shift) with (orand the humidity even surface-layer are curves a somewhat could systematic better be behaved identified. departure, in Temperature for this example case, but by not CO Sf 5 5 15 25 15 20 10 10 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 2 11638 11637 erent observation levels. Although the horizontal velocities in Fig. 12 are highly ff the Amazon forest Evidence from ATTO indicates that it is possible to associate the intermittent events Some evidence can be gathered from a spectral decomposition of the turbulent flow It is not yet clear what triggers these intermittent events. In general, previous studies A proper understanding of nocturnal vertical profiles and fluxes of scalars above any Gravity waves (GWs) maynights. Depending occur on in the magnitude the of the forest turbulent boundary drag, they layer influence the during exchange relatively calm is dominated by submeso processes,this such portion as of in the the flowFurthermore, that examples it determines in is the Figs. clear occurrence 12 from of theseexert and examples intense important 14, that wind controls it flow shear on patterns is episodes. the atthe exchange levels of height as scalars high variation at as of canopy 80 submeso m level.such flow Questions have as such yet as those to be planneddata answered. for to Tall this tower be observations, kind of carriedbetween analysis the on and canopy at to and deepen ATTO,the the are the Amazon understanding atmosphere very forest. of during important exchange the processes to calm provide nights the that4.2.5 are common Orographically in induced gravity waves in the stable boundary layer above at canopy level with the meanthe wind two shear intense above the events canopy. atof In 42 Fig. intense m, 14, wind around it is 21:30 shear evident and between that 02:00 42 LT, are and triggered 80 by m. episodes In conditions where the 80 m wind field nals are decomposed in terms(TKE) of spectrum their (Acevedo time et scaleas al., to a 2014), provide peak the a at more turbulent timeother intense kinetic scales hand, turbulence energy just there at greater is 42 than mlevel a 10 for appears sharp s scales energy (Fig. larger 13). increaseby than At at the 100 longer 80 s. large m, time wind Such making scales, direction apatterns this on variability that low-frequency the the apparent have flow in most been at Fig. recently energetic has 12. 80 classified m low These as intensity, is “submeso” are with (Mahrt, non-turbulent characterized large 2009). flow andally Submeso present apparently flow in unpredictable the temporal atmospheric variability. Itthe boundary is turbulent layer, becoming usu- scales dominant are in highlylayer. conditions reduced, when such as in the decoupled nocturnal boundary at the di in phase between 42 andhigher 80 m, at it is 80 m, clear from while this there plot that are the more wind speed turbulent is fluctuations generally at 42 m. When these sig- events that occur inof the turbulence decoupled variability generated state nearoccurrence have the of been surface the characterized (Costa as highest etat al., natural intensity the 2011). modes at canopy At level. 42occurrence? ATTO, m the Is indicates it that possible, intermittency then, to is identify generated the mechanisms that trigger their indicate that thelayer, more propagating from intense above (Sun events et are al., 2002, generated 2004). above On the the other hand, nocturnal less intense boundary et al., 2004). Thiscated is decoupling corroborated and by intermittency early occuring during observations more at than the half ATTO of site, the which nights. indi- forest canopy depends, therefore, ontent explaining turbulence the at atmospheric canopy controlsthere level. on are In intermit- the indications Amazon thatquence forest, turbulence of this is flow necessity more instabilities is intermittent generated enhanced, by there, as the possibly wind as profile a at conse- the canopy level (Ramos (Fig. 12, bottom panel).canopy During (42 this m) night, happened during the two majority specific of events, the at exchange around just 02:00 above and the 03:30 LT. As a consequence, ita is night. common The that example winds fromboth from the horizontal all ATTO site possible wind indicates directions components that42 occur despite are to in such generally the such a in large 80 mious phase variability, level. turbulent above Vertical events the velocity of canopy, atless variable from intensity the turbulent, the scattered 42 the m throughout 80 levelbehavior. m the The is night. level relevance highly is While of intermittent, the being alsoexchange with intermittent less becomes var- events intermittent, to clear characterize presenting when canopy-atmosphere a one more looks continuous at the fluxes of the scalars, such as CO 5 5 20 25 15 10 25 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | (8) (9) (7) is the Scorer L , measured in the T 90 m) and are available ∼ is the dimensionless gradient of the , and temperature, is second derivative of the wind speed w 00 θ/θ U z ∆ 11640 11639 , computed as z 2 /U > k 00 U is the mean wind speed, and 2 − U 2 θ/θ z is the gravity acceleration and is the wave number associated with the ground undulations and /U ∆ U/∂z g 2 2 k g ∂ N q = = 30 m) from the original spatial resolution of 3 arcsecond ( is the Brunt–Väisälä frequency, defined as: = Two kinds of data were used: topographic and meteorological. A digital topographic Time series of the vertical wind velocity and of the fast response temperature data Figure 15a shows a topographic image of the experimental site with colors ranging Fast response data of vertical wind velocity, 00 2 S ∼ image of the region surrounding theof experimental surface site undulations was and used their toysis scales analyze of the by features occurrence, complex as Morlet wellLocal wavelet as the transforms geomorphometric space-scale (Farge, anal- variables 1992;pographic were Thomas Mission) and derived data Foken, from 2005). (Valeriano,( 2008). the These SRTM data (Shuttleon were the Radar site refined. To- www.dsr.inpe.br/topodata/dados.php to 1 arcsecond provided by a sonicat anemometer a and height thermometer of weredata 81 m used was above to 10 Hz. the detect ground.anemometer Wind GWs The speed and events sampling and thermometer rate temperature60 measurements, of Hz vertical the for respectively, profiles both, measured with were making turbulence agradients it provided of possible sampling by to wind cup rate compute velocity the and of et Brunt–Väisälä the al., frequency, 2009). Scorer the Data parameter vertical from for fiveeach GW nights between have classification been Julian (Steeneveld analyzed, days consistingobservational of number 120 data 42 files available of and from 30 the 46 min time ATTO site. of between The 18:00 the analyses and year were 06:00 2012, LT, carried for each representing out night for the with the first availablefrom data blue (Fig. to 15). red representing the altimetry values in meters above sea level. The black virtual potential temperature. in relation to the height, U N N where nocturnal boundary layer (NBL)rence at of gravity the waves, ATTO and siteby to were identify terrain under analyzed undulations, which to using situationsOne detect they the of would the methodology be the occur- proposed generated goalswith by of the Steeneveld this conditions et study under al. is whichin (2009). to contrast GWs to would investigate those be the under forcednisms structure which by (class GWs of II). ground would turbulence To be undulations reach associated expected (class thison to goal, I) Chimonas be the and forced methodology Nappo by of (1989), other Steeneveldment has mecha- et belongs been al. used to (2009), to class based define I whether or a class specific II, measure- basedL on the condition: where parameter, processes that take place inet the al., stable 2009). boundary While layer convectivedriving of turbulence mechanism the decays is after atmosphere the nightfall. (Steeneveld main Asrelevant a factor in result, for the other daytime physical stable transport, processes boundaryvertical become this divergence layer of (SBL), radiation such (Drüeintermittency as and (Mahrt, Heinemann, drainage 1999), 2007; flow atmosphere–surface Hoch interactions (Sun (Steeneveld etand et et al., al., GWs al., 2007), 2008), (Nappo, global 2004), 1991;waves Brown and can Wood, be 2003; generated Zeriof by surface and roughness, several Sa, topography, forcing convection, 2011). terrainThese Internal mechanisms, undulations, features gravity including etc. can (Nappo, sudden reallocate 2002). energy changes ing and atmospheric momentum vertical and structure arenomena significant and (Steeneveld in the et determin- coupling al.,under of 2008, typical mesoscale 2009). conditions to Chimonas of microscalemean flow and phe- the resulting Nappo planetary in turbulence (1989) boundary at showed unexpected layer, that altitudes. GWs can interact with the 5 5 10 15 20 25 20 15 25 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | were approximately q , and T , w , u ). For the data at 81 m height, the q 11642 11641 ), and humidity ( T , the time scales of the CS are about 44 and 55 s, respectively. For the exhibit temporal scales around 46 and 29 s, respectively. For the two ), temperature ( q w w , u and and T u The results revealed that the CS time scale of the vertical wind velocity is often A study on the structure of atmospheric turbulence was performed at the ATTO site to the spectra of theAnother horizontal interesting velocity feature is than that to the theand temporal vertical scale scalars of velocity the for are CS low for considerablythose frequencies. both at the shorter 42 wind m, velocity for i.e., the thethe region data influence immediately above of measured the a forest at canopyturbulent high-pass appears signals 81 filter to m (Krusche be that and compared under removes Oliveira, with the 2004; Thomas lower and frequency Foken, oscillations 2005). of the smaller than the scaleslevels. This of can be the explained by horizontal the velocity fact that and the scalar the spectra scalar exhibit greater properties, similarity for both scalars, equal to 33, 26, 30 s, and 31 s, respectively. CS of height of 42 m the coherent structure time scales of structures were determined following the methodology(2005). proposed by Figure Thomas and 16 Foken showsvelocities the ( average duration of CS for horizontal and vertical wind under daytime conditions,developing with a the better understanding aim ofuneven of terrain their covered contributing vertical by and to primary temporalhumidity forest the variability data in over were detection central a obtained Amazonia. of very using Wind,42 sonic and temperature, CSs anemometers 81 and m and and above gas ground, as analyzers, specified installed in at the methods section. The scales of coherent cal simulation (Patton, 1997; Bou-Zeid etPorte-Agel, al., 2011), 2004; particularly Dupont in and the Brunet,itinkevich nocturnal 2009; et boundary Wan al., layer and 2013), (Durden et andthe al., (v) 2013; atmosphere implications Zil- (Steiner of et the existence al., of 2011; CSs Foken for et the al., chemistry 2012). of points on the axes intopography Fig. of 15b the represent terrain, the whereas GWbeen the events generated that gray by have points terrain been represent orography. inducedthe GW The by analyzed events results the situations that show have represents that not very GW a important induced considerable for by fraction the terrain of site, environmental undulations. studies as This that finding it are is indicatesdepend being that carried on some out the mixing atwind characteristics the characteristics direction. Uatumã of of the terrain nocturnal undulations boundary and layer 4.2.6 therefore change with Coherent structure the time scale aboveCoherent the structures ATTO site (CSs) are aflow, particularly ubiquitous phenomenon over in forests the (Hussain,immediately turbulent above 1986). the atmospheric They plant canopy, occur where thelike” in CSs shape the of associated the roughness with scalar sub-layer the signalsinteracting two-phase show a movement with “ramp- of the sweep canopy. and Coherentatmosphere ejection exchange of structures processes the play (Gao flow an andis Li, important some 1993; role Serafimovich consensus in et that al., biosphere– full CSs 2011). agreement are There on associated the with percentageFitzjarrald, turbulent of 1994; flows, the Thomas although and turbulent there Foken, fluxes is 2007;research associated Foken no with on et them al., the (Lu 2012). dominantThomas There and has and scale been Foken, of much 2005) occurrence andtion the of (Paw physical U CSs mechanisms et responsible (Collineau al.,panharo for and 1992; their et Brunet, genera- Raupach al., et 1993; 2008;devoted al., Dias to 1996; Júnior McNaughton the et and detection al.,2004) Brunet, of 2013). and 2002; Considerable CSs the Cam- research (Collineau dissimilarityand has and between scalars also CSs Brunet, (Li been associated 1993; and withstill Krusche Bou-Zeid, the poorly and 2011). transport known, However, Oliveira, of many particularly:manifestations momentum aspects (i) of of their their their interaction vertical occurrence with(iii) variability are gravity the (Lohou waves influence (Sorbjan of et surface and al., heterogeneity Czerwinska, on 2000), 2013), their (ii) features, (iv) the aspects of their numeri- 5 5 25 20 15 10 10 15 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | (10) . The V ), mea- n R ), above which λ V ). Classes (I), (II), 2 − , and equivalent black 4 , CH 2 concentration, temperature, or specific 2 ) is related to the mean wind velocity, 11644 11643 TKE changes greater than 10 Wm were measured with multiple instruments in par- V n e R 2 / 1 and BC i 2 w 2 σ + , is defined as: 2 v are the components of the zonal, meridional and vertical winds, σ represents the SD of each variable. TKE V + w σ 2 u ciently high sampling rate, which allows cloud detection (with passage σ . They are: (IV) cases where the net radiation induces organized move-  2 ffi ) was initiated at the site, which has been running almost continuously − e 2) , and / v , (1 , but is associated with occasional bursts of top-down turbulence. In Regimes 1 u h λ 10 Wm V = > We analyzed 53 data files from the wet season and 79 data files collected during the Cava et al.’s (2004) classification of nocturnal time series is based on the existence of The search of parameters to characterize the turbulent regimes of the nocturnal n TKE turbulent velocity, V turbulence generated by bulk shear instability,by defined as the the measuring mean wind height.than speed divided In Regime 3, the turbulence occurs at wind speeds lower allel (see Table 2)these an quantities. almost In November complete 2012, timeto the series include long-term since measurement measurements setup March ofaerosol was 2012 ozone, number upgraded is aerosol concentration. available scattering, Dueare for to aerosol a the size few complex distribution, larger logisticscomplete and data at from gaps this the in remote middle some of site, of May there 2013 these to time November series, 2013 but and the from datasets February are 2014 almost to and 2 the scale of turbulent velocity ( where carbon, BC up to the present. As CO 4.3 Measurements of atmospheric composition In March 2012, a basic set of measurements (CO, CO of clouds being identified by rapid respectively, and are represented by Cava’s classesFurthermore, I, during II, the and wet V seasonof the for classes both occurrence I wet associated and and V withturbulence dry show Regime seasons their turbulent 1 highest (Table Regime 4). prevails. percentage For 3.IV the and Class dry V season IV occur we most is observe frequently more that in turbulent situations frequent classes associated when with I, Regime 1 (Table 5). dry season at the ATTO site. Our results show that the prevailing conditions in the NBL sured at a su instability and modulated byshows strong the turbulence vertical and wind gradient speedturbulence exceeding of a increases threshold potential value temperature. ( systematically Regime with 2 increasing wind speed. This describes the a dominant pattern in scalar data, such as CO boundary layer is based onare Sun defined et as al. (2012). follows: The Regime three 1 turbulent shows regimes in weak the turbulence NBL generated by local shear 4.2.7 Characteristics of the nocturnal boundaryThe layer characteristics of theUatumã nocturnal River were boundary analyzed layer forologies: (NBL) the (i) at the wet thermodynamic and the classes the(ii) ATTO of site dry the the turbulence seasons, near NBL regimes based the proposed proposed on by by two Cava Sun et method- et al. al. (2004) (2012). and humidity. It also takes into account the variability of nocturnal net radiation ( (III), are defined bydisturb atmospheric the conditions stable boundary free layer of aboveby the the Cava forest. influence et The of al. classes clouds, (2004): arein defined which (I) scalar as the can time followed occurrence series; ofously (II) coherent occur the structures in presence in the of thegravity time sinusoidal form waves; signals series of (III) (“ripples”) of “ramps” the thatet scalars existence simultane- al. above of the (2004), turbulence canopy, “periods fineries and that structure which data”). lack are (i.e., The any typical according lastto geometric for to the two structure simultaneous Cava categories, or occurrence (IV) of periodicityR clouds in and and the (V), organized time movements ofments, with se- Cava and variations (V) et in those al.’s where classificationin the organized refer change movements. in net radiation is not correlated with changes 5 5 20 25 15 10 25 15 10 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | CO ratios are levels at ATTO / 4 4 record. CO does 4 and CO are shown in . 4 from three levels (4, 38, x 2 SD) and indicating a source at the ± , and CO are compared in Fig. 23 with 4 and CO show a nighttime accumulation 2 , CH exhibits a clear minimum during daytime at 2 -CO source is not known. A remote source 11646 11645 2 4 2.0 ppb (average concentrations. This suggests the presence of regional ± 0.5 ppb, which was lower than observed above the forest 4 ± CO peaks, we occasionally observe, mostly during nighttime, / 4 proceeds from above the canopy (Fig. 18). The origin of this behavior, , and CO 4 4 0.3 ppb). Measurements in the canopy (24 m) vary by a factor of ten from and CO at the ATTO site. CO ± 4 , CH and CO still exhibit a small vertical gradient below the canopy, indicating 2 peaks of up to more than 100 ppb amplitude. These peaks last a few hours, from June to August is about 5 ppm above the values during the months from 4 4 2 , CH 2 concentrations clearly reach lower values than at both upstream locations, re- and CO predominantly on the lowest measurement level. Examples are shown emissions in the airshed of ATTO. , CH 2 2 4 4 Monthly daytime concentrations of CO Statistics of monthly daytime 30 min measurements of CH Apart from these CH Figure 21 shows the statistics of monthly daytime (defined as between 13:00– Additional evidence for local surface sources are sporadic concurrent increases of several orders of magnitude higher than the values typical ofshort combustion CH emissions. 16:00 LT, or 17:00–20:00 UT) 30and min 79 m) measurements respectively. The of measurementsthe at CO the upper 4 m levels, level while are the consistently higher 38 m than level consistently shows lower values during daytime they do not always concur with“bursts” increases of in particles CO with concentrations, and a often diameter coincide of with a few tens of nanometers. CH a local source near the ground. in Fig. 20.(e.g., The from the origin large water of reservoirseems this behind unlikely, the as local Balbina such Dam CH a 60site. km signal A northwest would combustion of be ATTO) source vertically also diluted appears before unlikely, reaching as the the ATTO observed CH which seems to be linkedCO to multiple processes, is under investigation. During daytime mid-canopy level induced by photosynthesis. Interestingly,maximum the of build-up CH of the nighttime in the sub-canopy space andgradient, a which corresponding is steepening greatly of reducedthroughout the during vertical the daytime concentration canopy. due In to the addition, enhanced CO vertical mixing canopy top. During nighttime, thecanopy mixing light-driven ratio emissions fell of to 1.1 isopreneat cease 80 m and (2.3 the in- show a seasonal cycle atdry ATTO with months with concentrations a higher significant by about fraction of 50 ppb air during coming the from the south-east (see Fig. 3). CH The first successful verticalmeasured gradients in of biogenic Novemberdescribed VOCs 2012 and in total at Sect. OH(Fig. the 3.4. reactivity 24). were Under walk-up Diurnal daylight fluctuations tower conditions,24 m isoprene of using level, mixing reaching isoprene ratios the up were to are always gradient 19.9 highest apparent at system at the as all heights than the top levelyear. The (79 m). record This is still indicatesthat too that CO short photosynthesis to reveal is aDecember active clear to seasonality. throughout February. Nevertheless, it the appears Fig. 22 (from the 79 mof the level only). analyzer, a Because seasonal of cycle a is large not data discernible gap in due the to present a CH malfunctioning lie almost on Northernnorth Hemisphere of levels ATTO throughout in austral the winter year,with and even its the when site lower the is background ITCZ in CH is the atmospheric Southern Hemisphere 4.3.2 Biogenic volatile organic compounds and OH reactivity measurements upstream of ATTO: Cape Verde (greenend symbols) of reflecting the the southern Northern Hemisphere,conditions in and the Ascension Southern Island Hemisphere. (brownCO At symbols) least representing during the periodflecting of July the to regional December, carbon sink in the Amazon domain. Likewise, CH now. Furthermore, several intensive campaignssurements of were aerosol conducted properties, with VOC, additional OH reactivity, mea- and NO 4.3.1 CO Figures 17–19 show the diurnal cyclesof of CO the vertical distributions of the concentrations 5 5 25 20 20 25 15 10 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | . 1 − erent ff mixing 3 erent studies. ff et al., 1989; Andreae erent influences, high- ff ff , which is “stored” within cult. However, the mixing 3 ffi mainly controlled the mixing 3 maxima at the uppermost height 3 erent measurement periods or di ff et al., 1990; Andreae et al., 2002; Rummel ff 11648 11647 to exhibit distinct vertical profiles (Fig. 26), which 8 ppb, respectively. As found in previous studies, its 3 erent studies in the Amazonian rain forest are within 40 ppb in Rondônia: Kirchho ff ∼ erences were measured between 38 m (just above the ∼ ff di formation (Crutzen and Andreae, 1990). A site comparable 3 3 11 and ∼ mixing ratios (Fig. 26) show typical diurnal cycles for both seasons, with val- erent picture is observed during the dry season, with much higher O 3 ff mixing ratios measured at 39 m from 2009–2012 (Artaxo et al., 2013) match exactly In November 2012, the high levels of isoprene measured above the canopy con- During the wet season, the amplitude of the mean diurnal cycle at 79 m is only about A di 3 quality long-term measurements arethe required, ATTO project. which are now being generated within 2 ppb, whereas itserved is within 3–4 the ppb canopy during andThese the the variations understory dry can with up be season. to attributed The 5 to ppb highest (24 downward m) amplitudes mixing in of are the O dry ob- season. been used extensively in the pastO (Artaxo et al., 2013). Atthose the measured ZF2 at site, the mean ATTO site maximum forduring the wet the season, but dry areATTO about season. site, a This factor but of could may 1.5 also higher bebiogenic be emissions attributed related at to to the the sites. the In di more order pristine to distinguish character these of di the the canopy (so calledpleted storage by flux, chemical see reactions, Rummel mostly et with al., soil 2007). biogenic It NO, is and subsequently deposition de- after the to the ATTO site is the ZF2 site, located about 60 km north-west of Manaus, which has ratios at more pollutedet al., sites 2002; ( Rummel etcausing al., photochemical 2007), O which can be related to biomass burning emissions canopy) and the top of the tower at 79 m during the wet season. ratios near the surface,above with the only canopy. This aFurthermore, may minor only explain contribution small the from O similar photochemical mixing formation ratios in the di deposition to surfaces causesmakes a O direct intercomparison to other measurements di a narrow range ofet 7 al., to 2007; Artaxo 12 ppbWofsy et (Kirchho al., (1990) 2013) revealed during that the wet downward season. transport A budget of study O by Jacob and ratios above the canopy from di (79 m) are about ason, factor averaging of about 1.4 higher during the dry season than during the wet sea- tributed significantly (on averageit about can 85 %) be to seen the8 that ppb total median in OH isoprene the mixing reactivity. late From ratios afternoon Fig. of above 25, between the 0.5 ppb canopy give at an 06:00 LT OH and reactivity of about 1–20 s day to night, whileof measurements two. close This to clearlynoon, demonstrates the when a ground light canopy (0.05 and m) emission temperatureground of vary are level isoprene, only were at with by always their a the a maximum.relatively lowest, peak Isoprene factor slow indicating around mixing downward a ratios potential mixing. at sinkand A the at other detailed biogenic the discussion VOC soil/litter of at level ATTO or measurements was published of recently isoprene (Yañez-Serrano et al., 2014). The gap between the twoisoprene. curves For is most the of fraction thesurements. of time On total this two OH gap occasions reactivity istotal that within small OH is and this reactivity not within dataset was due the from significantlyin to uncertainty higher November the of than 2012, early the the however, mea- morning isoprene the noon (09:00 contribution, just LT) these coincident after being sunset with (17:00was a LT). the For drop major all sink in other for light OH timesreactivity above levels, in can the and be the canopy. Overall observed, course in a similar of distinct the tolifetime diel the that after- of variability day, of in OH isoprene its total radicals major OH during contributor,at isoprene. the The 80 dry-to-wet m median transition varied season fromwill above determine the about the forest 50 seasonal canopy ms variability byof in total isoprene. day OH to reactivity and 100 ms the relative by contribution night.4.3.3 Ongoing measurements Ozone profiles The O ues increasing from the morningdeposition to and the chemical afternoon reactions. and The subsequently afternoon decreasing O due to 5 5 25 15 20 10 15 20 25 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ob- a α could be a is very low, α a ) is often used σ values indicate a , which is much , with somewhat a , especially nitric 1 cients are similar a 3 − ffi g 2 1 indicates the aerosol ∼ a deposition due to enhanced values, reaching an average erences in å a 3 ff σ , is comparable to that of the scat- a σ 2.0 or greater (Bond et al., 1999). Our cients from both seasons, which aver- cient measurements at 637 nm vs. the ffi ∼ ffi a cient, ) has been calculated by applying an orthog- mixing ratios occurs at the canopy top. This ffi a 11650 11649 3 α ) and trace gases that react with O 3 erent light absorbing components of the aerosol to the ff reported previously for an Amazonian forest site (Gilardoni 1 − g 2 on average. The absorption Ångström exponent (å 1 − during this period. In contrast, during the wet season, ) averages 1.25 during the wet season, lower than the 1.62 obtained for 1 s cient. The regional transport of biomass burning emissions, most important − ffi cients reach their minimum values, however, some episodes of long-range trans- ffi The seasonality of the absorption coe The mass absorption cross section ( The contrast between the wet and dry seasons can be attributed to a combination of 3.46 Mm tained for the 2013–2014 wet season measurements was 13.5 m around 0.52 Mm to estimate the composition of light absorbing aerosols. An å higher than the 4.7 m et al., 2011), measured also during the wet season. The high apparent tering coe between August and October, produces a rise in the refractive BC (rBC) mass concentrations measured by the SP2. The average is in the Rayleightherefore regime, wavelength and independent the (Moosmüller absorption etthe al., is 2011). presence dominated Higher of by å additional soot-likeand light carbon absorbing Gelencsér, and material, 2006). is like Thisbiomass brown kind burning carbon of aerosols, (BrC) yellowish usually (Andreae hasmeasurements or an show brown å only organic relatively material,higher minor abundant values seasonal in during di thethat wet soot season carbon (1.53) is thanyear. an in The important the contribution contributor dry of to the seasontotal aerosol di (1.40), observed light suggesting aerosol absorption absorption throughout is the currently being investigated. onal regression to the MAAP absorption coe explained by the facttechnique that did the not SP2 sizelikely account related dynamic for to range rBC an wasor enhancement particles 70–280 nm to of larger and the light than presence absorption thus of 280 by the nm. coatings additional However, on light-absorbing it the substances rBC is besides particles, rBC. also Our prelim- (mostly primary biogenic particles)large during seasonal the variability wet of season,less the because intense seasonal in submicron changes. contrast particles, to the the supermicron fraction shows forest canopy becomes decoupled from thewet atmosphere season, above at the nighttime. largest During the decrease in O might be attributed tostomatal aperture a during lower the wet canopybe season resistance the as proposed subject to by of O Rummel futurebetween et turbulence work. al. (supply Further (2007) of and investigations O will will also focus on the interactions port of aerosols from the ocean and Africa stillof lead to higher episodically removal elevated values. ratesinfluence from by biomass wet burning and depositionare fossil during fuel the emissions the main during wet theexponent sources dry season (å of season, and which submicron thethe particles dry dominant season. at This behavior that results from time. the high The relative proportion scattering of larger Ångström particles oxide (NO). 4.3.4 Aerosol optical properties The aerosol optical properties measuredand at summarized ATTO are in shown Table as 6. a TheOctober, time averages and series were calculated in the for Fig. the 27 wetments dry season, season, and August– February–May 2013 (2012–13these for for two the the seasons are scattering absorption nottween measurements). measure- included the cleanest in The and the transition “more summary,to in polluted” periods those periods. order reported between The to by scattering show Rizzo(60 coe the et km contrast al. N of be- (2013) Manaus). from Thesource measurements regional of performed transport particles at of during the biomass the ZF2comparing burning dry site emissions season. the is Its scattering influence the and is main age significant, absorption about as coe 3–6 can be times seen higherseason, by during ATTO is the meteorologically dry located thancoe in during the the NH wet and season. the During scattering the and wet absorption 5 5 10 15 20 25 25 10 15 20 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 70 nm) ∼ erences in . A charac- ff 3 − man et al., 2012). ff ), implemented by the MAAP in 1 − g 2 (6.6 m a erent instruments, which are based on optical and aerosol size spectra reveal the character- 11652 11651 α ff 3 − 150 nm) modes are separated by the so called Hop- ∼ 70 nm). ∼ 110 nm), which is thought to be caused by cloud processing (e.g., ∼ 140 nm) shows the highest relative increase and therefore partly “swamps” ∼ erent sizing techniques. Integrated particle number concentrations agree with mea- Besides the Aitken and accumulation modes, which dominate the total aerosol num- During the dry season, the dominant wind direction is E to SE (Fig. 3), which brings The pristine conditions that prevail at the ATTO site during the wet season, when At the ATTO site, the atmospheric aerosol burden shows remarkable di The wet season is characterized by clean air masses from NE directions (Fig. 3), ff Autofluorescence based techniques (e.g.,sor, WIBS-4A) the have Wideband become Integratedaerosol an Bioaerosol particles established (FBAP) Sen- approach in to online probe measurements (Kaye fluorescent et biological al., 2005). Figure 31 shows assumed to dominate the coarse mode (Pöschl et al., 2010; Hu ber concentration, acounts persistent for coarse a mode significantpeak fraction is occurs of throughout observed the the year, at total withthe aerosol higher about absence abundance mass 3 of in µm, (Fig. the long-range dry 29). which transport, season The ac- primary (Fig. coarse 29). biological mode In aerosol particles (PBAP) are teristic dry season size spectrumcle is concentrations across illustrated the in entire Fig. sizeimum 29, range. Typically, the at which accumulation shows mode increased (max- parti- the Aitken mode (shoulder at season aerosol number concentrations typically range from 500–2000 cm polluted air from urban sources and deforestation fires in SE Brazil to the ATTO site. Dry pel minimum (at aerosol volume distribution clearly indicateswhich a increases large the enhancement integrated ofmagnitude particle coarse (Fig. 30b). particles, volume concentration by almost one order of Zhou et al., 2002; Rissler et al., 2004; Artaxothe et aerosol al., 2013). concentrations are remarkablybiogenic low sources, and are controlled bySaharan episodically local dust, interrupted and/or and/or African by regional biomasset long-range burning al., aerosol 2010a, transport b; (e.g., Baars of Talbot et etseason sea al., al., size 2011). 1990; spray, Figure distribution Martin 30 during displays selected characteristicTypically, the episodes changes in with aerosol the long-range abundance wet transport insubstantially intrusions. the increased accumulation and and the coarse Hoppel mode minimum size almost range completely is disappears. The inary results indicate that the constant and electromobility sizing. It confirmsdi the overall consistency and comparability of the istic “wet season shape”. Atrum representative example is is characterized shown in bymodes Fig. a as 29. 3-modal The well size shape as spec- with a noticeable pronounced coarse Aitken mode and maximum. accumulation Aitken (maximum at surements by the backup CPC withinthe 15 main %. The aerosol sample inlet airaerosol has scattering, at been absorptivity, collected 60 hygroscopicity, m and through chemical height, composition. which is also used for instruments measuring which result in ations pristine typically atmospheric range state from at 100–400 cm the ATTO site. Total particle concentra- order to retrieve theproperties BC of mass Amazonian aerosol concentration, particles. is not representative4.3.5 of the true Aerosol optical number concentrations and sizeContinuous distributions measurements of aerosolducted particle at size the and ATTO site concentration sinceinstrumentation have March has been 2012. been con- Over increased theaerosol stepwise last size years, to and the provide concentration extent uninterrupted time of series.ment and the intercomparisons, Figure redundant sizing including 28 four shows di one of the frequent instru- terms of size distribution andplays concentration the depending average on particle theMay number seasons. 2014) and Figure and volume 29 size dry dis- cusses distributions season on for (13–20 SMPS typical and September OPS wet 2014)to measurements, (6–13 10 covering conditions. µm. an The aerosol comparison size range fo- from 10 nm and accumulation (maximum at 5 5 20 25 15 10 10 25 20 15 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 3 + 2 − cm 3 and NO + 70–80 % in the ∼ 11654 11653 (40 % of the concentration of supermicron parti- was measured for up to 10 elements by EDXRF 3 of total Fe) was found. The soluble (and therefore − 3 2.5 − aerosols were analyzed. A soluble fraction of only 1.5 % 2.5 10) when this ion is in organic forms, and low (2–3) when ∼ Fe(III) of 120 ngm 3 − To explore the bioavailability of important trace elements, the oxidation state and sol- The bulk composition of PM Sulfate comprised 12 % of the mass concentration measured by the ACSM followed The time series of aerosol concentrations and the average chemical speciation are (1.8 ngm bioavailable) fraction of Fe is ancles, important with impact parameter in on the the2009). overall phosphorus biogeochemical cycle cy- and biomass production (Liptzin and Silver, ubility of iron (Fe) in the PM analysis on a set of samplesabundance obtained of in crustal March/April elements, 2012. Thetransport illustrating analysis one from showed exemplary a Africa high episode (Fig. ofinfluenced 33). long-range by dust Back dust trajectories transportand indicate from particularly that Africa, this pronounced which period1992; in is was Ben-Ami March a indeed et and phenomenon al., Aprilespecially observed 2012). during (Prospero annually Local the et sources wet season, al., ofof because mineral mineral 1981; of dust dust Swap the aerosols aerosol wetness et duringthe of can al., the the North be soils. wet excluded, African The season, prevalence when desertstransatlantic airmass to dust trajectories the plumes reach by Amazon from observed lidar, Basin, crustal is elements. in strong combination evidence with for observations the of long-range origin of the is expected to bein large inorganic ( forms, suchLarge as values for ammonium this nitrate ratiopresence (Alfarra were of often et organic observed al., nitrate. during 2006; Elevated thisa concentrations Fry period few episodes, of and et when chloride may this al., were indicate speciesulate observed 2009). the represented mass, up during which to is 13 % consistent ofsalt, with the going earlier total back observations submicron to of partic- the long-rangeof ABLE-2B transport this campaign of (Talbot species sea et still al., requires 1990). further Because analysis, quantification the results are not shown here. (main nitrate fragments measured by the ACSM at mass-to-charge ratios 30 and 46) the FBAP number and volumesite, size which distributions are from in the goodbutions WIBS agreement are operation with dominated at the in the OPS number ATTO peak by measurements. a The from narrow FBAP 2 peak size to at distri- number 5 2.7 µm µm concentration and (Fig. in is 31). volume For by 0.22cles), cm particles a and broad larger the than 1 corresponding µm, the volume mean concentration integral is FBAP calculated to be 3.0 µm nium sulfate, there isform some of organic indication nitrate. that This part is because of the the ratio between nitrate the could fragments NO be present in the by ammonium (5 %), nitrate (4that %) and the chloride aerosol (2 %). was The mostly ionic neutralized. mass balance While indicated sulfate is mostly in the form of ammo- (62 %). The ratio ofdependence, FBAP starting to total from particles 10 % (number at concentration) 1 shows µm a and clear rising size to a peak value matter dominating (78 %) the aerosolminor composition contributions and (Chen inorganic et ions al., making 2009; relatively Pöschl et al., 2010; Artaxo et al., 2013). given in Fig. 32.chemical The average speciation concentration is of in non-refractoryconducted relatively aerosols, at good as agreement the well with ZF2 as previous site the wet during season AMAZE-08 studies (ca. 140 km SW of ATTO), with organic March 2015. For the continuous determination offrom aerosol composition, the a shared samplecomposition air aerosol is stream determined inlet is using taken (60 an m)was Aerosol installed and Chemical in Speciation the Monitor February (ACSM) 2014 non-refractoryThe that with data submicrometer the reported objective aerosol here of were making taken long-term during measurements. the early wet season transition from 1 to 31 size range of 3–10 µm. 4.3.6 Aerosol chemical composition 5 5 25 10 15 20 25 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , whereas the concentration of 3 − 10 weight %). “Biogenic” particles occur in < 11656 11655 was measured for terpene oxidation products 3 − -bond signals) and organic coatings of variable thickness. The spec- π . 3 − With single particle analysis, important information was obtained concerning the con- As mentioned in the previous section, the biogenic background aerosol in the wet A median concentration of 102 ngm tribution from organic aerosol particlesticles. The and majority the of agglomeration particles ofof in various S the types and fine of fraction K. par- containing consist This particles of observation organic from matter corroborates primary withorganic that emissions traces material can small (Pöhlker act et biogenic al., as potassium 2012). seeds and for sulfur- the4.3.8 condensation of Chemical composition of secondary organic aerosol and K. Irregular crystallizedparticles. particles Soot with particles Na, can Mg, bethe S, elements distinguished O, C by and and their C O. morphology, are and classified always contain as “salt” in the aerosol sampledpene over and the sesquiterpene Amazonber oxidation rain 2012 products is forest. shown in The in ambientpart Fig. concentration 36. of aerosol of Monoterpene the collected oxidation monoter- terpene products inshowed oxidation accounted much products, Novem- for lower the whereas concentrations. major the Onreached sesquiterpene average the oxidation about sesquiterpene products 10 oxidation % products on of some the days monoterpeneproduct they concentration. oxidation were The product even monoterpene as concentration,during oxidation November high however, products ranging as showed between a 26 23 % high and of variance 146 ngm the total monoterpene oxidation sesquiterpene oxidation products stayed quite constantof around 8 a ngm median concentration 5 Summary and conclusions Our initial ecological studies havebiodiversity, shown containing the forest ATTO site and to wetland be ecosystems located that in are an representative area of of many high clustering reveals the abundancetower of in the this various season particle (Tablecal 7). types interactions, In particles observed order were at tochemical classified the determine composition. into They ATTO the representative are sources classified groups as andinant, according “mineral” possible and when to chemi- Al, also their Si, contain O, minor andas Ca elements being are “organic”, like dom- when K, the Na,when concentrations Mg, of they and C also Fe. and contain Particles Othe are some in larger identified the P size particles classes; and they are S have similar smooth and ( boundaries and always contain C, O, S, N, P, season (i.e., Februaryevents. Statistical to analysis April) of the is electron episodically microscope (EPMA) superimposed results by by hierarchical transatlantic dust (SOM) (Pöhlker et al.,pyrogenic 2014). aerosols at These the observationswhen ATTO underline site biomass during burning the is the dominanceprevail absent dry in of and season. the aged undisturbed region, During biosphere–atmosphere the theprimary interactions aerosol rainy biological population aerosol season, is particles dominated (PBAP), byet biogenic biogenic SOA, al., aerosol, and 2012). such biogenic as salts Figureaerosol (Pöhlker population. 35 displays STXM elemental maps of this typical rainy season tral signature of the organic coating is characteristic for secondary organic material 4.3.7 Microspectroscopic analysis of single aerosolThe particles microspectroscopic analysis ofthe aerosol aerosol samples population at can a besurements given seen at time. the as In combination ATTO a site, withinto “snapshot” single the the of particle long-term highly aerosol characterization mea- variable providesFig. detailed aerosol 34 insights cycling displays in theanthropogenic the STXM-NEXAFS pollution, rain analysis collected forest at of ecosystem.crospectroscopy the an As reveals ATTO an a aerosol site example, substantial sample duringcores fraction with (strong the of substantial dry internally season. mixed X-ray particles mi- with soot 5 5 10 15 25 20 25 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , 2 ects of ff at five heights 4 en Schmidt, Alcides ff , CO, and CH 2 . The challenge for the future will 2 11658 11657 , this reflects the secular increase in concentrations as 4 . Ozone, VOC, and OH reactivity measurements indicate an 4 and CH 2 ce of Basic Energy Sciences, of the US Department of Energy under We thank the Max Planck Society and the Instituto Nacional de Pesquisas ffi ects of photosynthesis and respiration on the vertical distribution of CO ff ce of Science, O Continuous measurements of the carbon gases CO Overall, our measurements at ATTO support the view that there is no longer any The Amazonian aerosol is strongly influenced by seasonal variations in airmass ori- During 2015, we expect that many measurements will be relocated from the 80 m ffi surements of long-lived tracebe gases, to especially maintain CO these measurementssecular over trends the in coming decades, atmospherictem. so composition that and they can the reveal health of theAcknowledgements. Amazonian ecosys- thanks CAPES for his Ph.D.search grant. grants Maria (PELD-Project, Teresa F. Process Piedade 403792/2012-6).O thanks The CNPq ALS and is FAPEAM supported for re- by the Director, da Amazonia for continuousMinistry of support. Education We andda acknowledge Research Ciência, (BMBF the Tecnologia e contract support Inovação 01LB1001A) (MCTI/FINEPzon by and contract State 01.11.01248.00) the the University as Brazilian German (UEA), well Ministério as FAPEAM,thanks Federal the LBA/INPA CNPq and Ama- for SDS/CEUC/RDS-Uatumã. his Productivity Leonardo in Sá Research Grant, Process 303728/2010-8. Cléo Dias-Júnior Contract DE-AC02-05CH11231. We thanksynchrotron the radiation Helmholtz-Zentrum beamtime BerlinA. at for L. the BESSY D. allocation II. Kilcoyne of especially We for thank their also all constant thankproject, the support M. in people during Weigand, particular involved the M.Camargo Thomas in beamtime Ribeiro, Bechtel, Disper, the sessions. and Andrew and Hermes We technical Crozier, Bragaof would and Uwe Xavier. the like We INPA/LBA logistical Schulz, for acknowledge to their Ste the supportthanks collaboration micrometeorological of to concerning group Antonio the the meteorological Huxley ATTO Angelis parameters, and with and Leonardo special Sachin Oliveira. The S.and aerosol G. Gunthe team Glaßer for thanks (Max-Planck-Institute their forwith Isabella help Polymer Hrabe SEM Research, with de Mainz, imaging. instrument Germany)This We maintenance for paper kind thank and contains support Tracey results I.Agreement W. of Lieberwirth Andreae research between conducted for under theof help the Amazonas, National with Technical/Scientific Cooperation and copyediting Instituteresponsibility the the of for Max-Planck-Gesellschaft the manuscript. authors e.V.; Amazonian and the not Research, opinions of the the expressed participatingThe are State institutions. article the processing University entire charges forwere this covered open-access by publication the Max Planck Society. regions in the central Amazon Basin.temperature, The and meteorological wind measurements conditions reflect rainfall, typicalrainfall of and the airmass region, origins, with butmicrometeorological they pronounced also seasonality studies show in have substantial characterized interannualcoupling variability. the Early with nocturnal the boundary overlyingboundary layer atmosphere, and layer, the and its properties the formation of of turbulence orographically structures induced in gravity the waves. reveal the e place on Earth that canand be considered aerosol truly concentrations pristine. Evenlived show at species, this the like remote CO impact site, trace of gas anthropogenic emissions. For long- which are characterized bytion low of particle organic number matter. concentrationsbring Also and Saharan in a dust this and very season, Atlantic largedominant marine episodes frac- aerosols airmass of to intense source the site. transatlantic regionsfossil During transport fuel lie the combustion dry to result season, the in the substantial east production and of southeast, pollution aerosols. where biomass and gins. In theundisturbed rainy rain season, forest, there when are airmasses long periods come when from natural, biogenic the aerosols northeast prevail, across almost the presence of aepisodic source sources of of CO CH atactive the photochemical forest cycle floor, in andozone. the yet tropical unidentified boundary intensive layer and and a strong forest sink for a result of global emissions. For shorter-lived trace gases and aerosols, the e towers to the 325 m tall tower. This will significantly enlarge the footprint of the mea- regional sources and longthough range they may transport be can very be small during detected the almost cleanest at periods. all times, even 5 5 10 15 20 25 30 20 15 10 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | t, T., Moss, C., Scheidt, P., ff 11660 11659 , A., German National Committee on Global Change Research, Bonn, 59–66, ff carbonaceous aerosols, Atmos. Chem. Phys.,2006. 6, 3131–3148, doi:10.5194/acp-6-3131-2006, Esteves, J. L., Gash,Meixner, J. F. X., H. Nobre, C.,Valentini, R., A. Grace, von Jouanne, D., J., J., Nobre, Kabat, andenergy, trace Waterloo, C., gases P., M. and Lelieveld, Ruivo, J.: aerosols Biogeochemical J., in M.Res., cycling Amazonia: Malhi, the 107, d. of LBA-EUSTACH 8066, carbon, experiments, Y., L. 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G., von Randow, C., Sam- Wittmann, F., Householder, E., Piedade, M. T. F., de Assis, R. L., Schöngart, J., Parolin, P., Zeri, M. and Sa, L. D. A.: Horizontal and vertical turbulent fluxes forced by a gravity wave event Zhang, K., Castanho, A. D. d. A., Galbraith, D. R., Moghim, S., Levine, N., Bras, R. L., Coe, M., Zhou, J., Swietlicki, E., Hansson, H.-C., and Artaxo, P.: Submicrometer aerosolZilitinkevich, particle S. size S., Elperin, T., Kleeorin, N., Rogachevskii, I., and Esau, I.: A hierarchy of Wang, X., Piao, S., Ciais, P., Friedlingstein, P., Myneni, R. B., Cox, P., Heimann,Williams, M., Miller, C. J., A., Scanlon, T. M., and Albertson,Williams, E., J. Rosenfeld, D., D.: Madden, N., Influence Gerlach, J., of Gears, N., surface Atkinson, heterogeneity L., Dunnemann, N., 5 5 10 10 15 20 25 30 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | INPA, EMBRAPA INPA, EMBRAPA INPA, EMBRAPA INPA, EMBRAPA INPA, EMBRAPA MPI-BGC, MPI-C INPA, MPI-C, UEA MPI-C, USP, INPA MPI-C Height [m] 0.1; 0.2; 0.3;1.0 0.4; 0.6; 26.0; 19.0 1.0 81.0; 73.0; 55.0; 40.0; 36.0; 26.0; 12.0;1.5; 0.4 4.0; 81.0; 46.0 1.0 4.0; 24.0; 38.0;79.0 53.0; 0.05; 0.5;24.0; 4.0; 38.3; 53.0; 79.3 12.0; 0.05; 0.5;24.0; 4.0; 38.3; 53.0; 79.3 12.0; 0.05; 0.5;24.0; 4.0; 38.3; 53.0; 79.3 12.0; 60.060.060.060.0 MPI-C MPI-C 60.0 USP 60.0 60.0 USP 3.0 MPI-C 130130130 80 81 325 Base elevation [m] 11684 11683 W W W 0 0 0 S S S 0 0 0 USA) UK) Austria) trometer Scientific, USA) IRGA (LI-7200, LI-COR Inc., USA) Inc., USA) ment Technologies Inc., USA), TEIUSA), 49i IRGA (Thermo 7000 Electron (LI-COR Corp, Inc., USA) Scanning Mobility ParticlePaul, Sizer MN, (SMPS, USA; TSI size range: modelOptical 10–430 nm) Particle 3080, Sizer St. (OPS,10 TSI µm) model 3330; sizeWide range: Range 0.3– AerosolTechnik, Ainring, Spectrometer Germany; size (WRAS, range: 6 nm–32 Grimm µm) Aerosol Technologies, USA) USA) Ecotech Aurora 3000; wavelengths 450, 525, and 635 nm ment Technologies, USA) 59.992 00.033 00.335 ◦ ◦ ◦ 08.647 08.602 08.752 ◦ ◦ ◦ 58 59 59 (WGS 84) O mixing ratios CLD 780TR (Eco Physics, Switzerland), BLC (Droplet Measure- 2 , and H 2 , CO 3 and CO mixing ratios G1301 (CFADS-109) and G1302 (CKADS-018; both Picarro ,O 4 2 , CH 2 Overview of (micro)-meteorological sensors, trace gas and aerosol instrumentation Location and specifications of the towers and masts at the ATTO site. O molar density IRGA (LI-7500A, LI-COR Inc., USA) 2 and H Triangular mastATTO Tall Tower 2 2 Towers/mastsWalk-up tower Coordinates 2 2 QuantitySoil heat fluxSoil moisture Instrument Heat flux sensor (HFP01, Hukseflux, Water Netherlands) content reflectometer (CS615, Campbell Scientific Inc., 0.05 INPA, EMBRAPA, MPIC Height a.g.l./depth [m] Institution Soil temperatureShortwave radiation (incoming and reflected)Longwave radiation (atmospheric and terrestrial)PAR (incoming and reflected)Net radiationUltra violet radiationRainfall Pyrgeometer Pyranometer (CGR4, (CMP21,Kipp Kipp &Air & Zonen, temperature Zonen, Netherlands) and Netherlands) relative humidityAtmospheric pressureWind speed and direction 75.0 75.0Wind vector components Quantum (u, sensor v, w) Thermistor (PAR LITE, (108, Kipp Campbell & Scientific Zonen, Inc., Netherlands) USA)CO Termohygrometer (CS215, Rotronic MeasurementVertical profile Solutions, of CO 75.0 UV radiometerVertical INPA, (CUV5, EMBRAPA profile Kipp INPA, of EMBRAPA & NO, Net Zonen, NO radiometer Netherlands) (NR-LITE2, Kipp & Zonen, 0.1; Netherlands) 0.2; 0.4Vertical profile of VOCs Barometer (PTB101B, 3-D Vaisala, 2-D sonic Rain Finnland) sonic anemometer gauge anemometer (Windmaster, (TB4,Vertical Gill (Windsonic, Hydrological profile 75.0 Instruments Gill Services of Instruments Ltd., USP total Pty. 75.0 UK) Ltd., Ltd., reactivity UK) Australia) to OH 81.0; INPA, EMBRAPA, MPIC Black 46.0; carbon 73.0; equivalent 36.0; 65.0; 81.0 4.0; 50.0; 42.0; INPA, EMBRAPA INPA, EMBRAPA 75.0 Comparative Reaction INPA, EMBRAPA Method, Proton Transfer Mass Proton Spec- Transfer Mass Spectrometer (PTR-QMS 500, Ionicon, INPA, EMBRAPA Multi Angle Absorption Photometer (model 5012, Thermo- Refractory black carbonBlack carbon equivalentAerosol scatteringAerosol number concentrationAerosol size distribution Single Particle Soot Photometer (SP-2, Droplet Measurement Primary Biological Aethalometer Aerosol Particles (model (PBAP)Aerosol AE31, chemical composition Magee Condensation Scientific particle counter Corporation, (model 3022A,TSI, USA) Nephelometer (model 3563, TSI, USA) Ultra-High Sensitivity Aerosol Spectrometer (Droplet 60.0 Measure- Wideband Integrated Bioaerosol Spectrometer (WIBS-4, DMT) 60.0 Aerosol Chemical Speciation Monitor (ACSM, Aerodyne, USA) MPI-C 60.0 MPI-C USP Table 2. installed at the walk-up tower. Table 1. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 3 ) 13 13 26 12 1 − ± ± ± ± Carbon stock in m) and wood ) (Mg C ha 1 H 2 25 170 27 101 52 79 24 74 − ± ± ± ± ). 5 340 8 202 ρ 18 158 12 148 ± ± × ) (Mgha ± ± 1 H − × 2 ln(DBH × ) (spp. ha 1 0.9894 2.7 137 1.6 127 2.4 35 5.9 64 − + 0.64 m. ± ± ± ± ha ± 2 2.9205 − = SD (max) AGWB 0.62 m; plot 3: 1.81 0.4 28.9 0.1 23.6 0.9 27.6 2.0 22.8 4.6 (40)4.3 (38)4.4 (36) 26.4 28.6 31.7 132 142 137 318 335 368 159 168 184 3.0 (30)3.3 (32)3.5 (38) 22.7 22.6 25.4 135 120 126 181 194 232 91 97 116 3.8 (27)4.2 (29)1.9 (18) 26.8 25.8 30.3 26 49 31 126 146 173 63 73 87 4.7 (34)3.6 (26)5.0 (33) 24.3 16.3 27.8 82 46 65 190 98 185 95 49 93 ± ± 11686 11685 ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± Wet Dry Avg. Avg. 1.06 m; plot 2: 3.12 ± SD (max) Mean 0.8 20.7 0.2 14.8 1.5 13.1 1.5 11.4 13.9 (152)12.0 (120) 20.5 12.5 (96) 20.4 21.1 11.2 (100)12.7 (117) 14.9 14.6 (177) 14.8 14.8 8.1 (136)12.0 (78) 12.2 9.4 (117) 10.5 11.5 12.1 (90)10.4 (83) 15.2 17.7 (162) 11.2 12.9 ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± Mean IIIIII 46.8 %IV 14.0 % 49.1V % 28.3 7.6 % % 47.9 % 3.8 21.2 % % 45.7 % 7.6 27.8 % % 3.7 5.9 % % 11.3 % 7.6 % 3.75 % 19.6 % 29.2 % 18.2 % 1 % Class ATTO Duke ) (cm) (m) (m 1 65 21.3 17 20.9 − 195 19.4 150 18.5 ± ± ± ± Density DBH Tree height Basal area Species richness AGWB (Treesha ) as independent parameters (Feldpausch et al., 2012): AGWB 3 − 1 in gcm ρ Tree species richness, forest structure, above-ground wood biomass (AGWB) and Percentage of occurrence of Cava’s classes for dry and wet season obtained at the sd 597 sd 497 sd 721 sd 616 ± ± ± ± The carbon stock was estimated by 50 % of the AGWB (Clark et al., 2001). Aboveground wood biomass (AGWB) was calculated using a pantropical allometric equation considering diameter (DBH in cm), tree height ( Mean flood height in the igapó floodplains: plot 1: 3.40 Terra firme plot 1plot 2plot 3Mean 522 644 21.3 624 20.5 22.1 Ancient fluvial terrace plot 1plot 2plot 3Mean 516 483 20.9 492 20.8 21.1 plot 1 695 19.5 Floodplain (igapó) plot 2plot 3Mean 540 928 20.9 17.9 Campina/campinarana plot 1plot 2plot 3Mean 560 503 20.1 17.2 786 18.3 3 2 specific gravity ( 1 Table 4. ATTO site and a comparison withUSA. the results found by Cava for the Duke Forest, North Carolina, carbon stocks of the inventoried forest plots. Table 3. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 7.4 6.5 5.3 0.71 1.25 0.36 a b 8.0 6.4 4.8 1.25 0.52 1.53 13.5 15 11 8 0.26 2.32 0.26 a 31 Dry seasonMean Wet season SD Mean23 SD 15 1.62 3.46 1.40 700 nm 450/700 637 nm 470/960 637 nm 11688 11687 0.92). = 2 R ) 1 − Regime 1 Regime 2 Regime 3 g Wet Dry Wet Dry Wet Dry 2 ,m cient cient 450 nm a ffi 0.99). α ffi ) > ) s a 2 R ) ) 550 nm 1 1 Class I 19.2 % 49 % 38.5 % 16 % 42.3 % 35 % − − Class V 25 % 50 % 25 % 27 % 50 % 23 % Class IV 100 % 67 % 0 % 0 % 0 % 33 % , Mm , Mm s a σ σ Calculated by a log-log linear fit including the last sixObtained wavelengths measured by by orthogonal the regression ( Scattering coe ( Scattering Ångström Exponent (å Absorption coe ( Absorption Ångström Exponent (å Mass absorption cross-section ( Distribution of Cava’s classes associated with the turbulence regimes for the ATTO Summary of aerosol optical parameters for the dry and wet seasons. Average and SD Aethalometer ( b a Table 6. are calculated from 60 min data. Table 5. site nocturnal boundary layer. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 40°W

60°W Uatumã São Sebastião Sebastião São do

° 0 S 20°S

Itapiranga Itapiranga Silves Itacoatiara RDS RDS Uatumã 11690 11689 ATTO ATTO 13 km 13 Porto ATTOPorto Porto Morena Vila de Balbina Balbina de Vila 50 km 0.5 700.5 13 420.5 17 58 820.5 0 0 6.1 72 0 3 0 28 0 9.1 0 0 0 0 0 0 0 0

1.02.0 0 241.02.0 27 60 28 501.02.0 32 71 37 47 5.3 01.02.0 1.2 8 1.7 27 16 41 79 34 0 0 0 6.7 13 36 31 21 0 0 17 16 21 0 0 17 0 13 0 2.4 5.7 0 0 0 0 0 0 11 ∼ ∼ ∼ ∼ ∼ ∼ ∼ ∼ ∼ ∼ ∼ ∼ Rio Preto Rio Eva da 0.5 1.0 0.5 1.0 0.5 1.0 0.5 1.0

Manaus Manaus 101 km km 101

174 - BR Location of the ATTO site. The main map shows the access to the site via the road Presidente Presidente Figueiredo Relative abundance of single particle types obtained at the top of the walk-up tower in 16 0.25 17 0.25 18 0.25 DateApr 2012 (µm)1 Size fraction Organic 0.25 with S,K Organic Mineral Biogenic Salts Soot and riverboat connections. (Background map from Google Earth.) Figure 1. Table 7. April 2012 (in %). Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | (from: Gridded 2 grid resolution (Kaiser ] ◦ -2 -2 10 Jun 2014 Sep 2014 Dec 2014 Mar 2014 -3 10 -4 10 0.1 % (cyan). Monthly fire map de- -5 Fire rad. power [W m > 10 (dark red) persons per km Feb 2014 May 2014 Aug 2014 Nov 2014 + 1 % (blue), 11691 11692 > 40 0 Jul 2014 Oct 2014 Jan 2014 Apr 2014 Longitude -40 10 % (green), > -80 0

60 40 20

-20 -40 -60 Latitude Back trajectory frequency plots and satellite fire maps for ATTO site in 2014. Back Land cover and population density map of northern South America. The land cover Figure 3. trajectories (9 days) have1000 m) been (Draxler calculated and with06:00, Rolph, 12:00, HYSPLIT 2015). 18:00 (NOAA-ARL, UTC) Four – back GDAS1,coding frequency trajectories of start plots have frequency are height been based plots: initiated on monthly per trajectory day ensembles. (0:00, Color Population of the World, Version 3ence (GPWv3) Information provided Network by (CIESIN), the Columbia Center University). for The International ATTO site Earth is Sci- marked by a star. map (GlobCover 2009, downloaded from: http://www.esa-landcover-cci.org/,and 11 July UCLouvain) 2014, highlights ESA vegetated areasevergreen in forest, green and tones mixed (deciduous(regularly broadleaf forest, flooded broadleaf and and forest, needleleaf permanently forest) floodedsity areas). and map) Populated span water areas a bodies range (given from as in one population blue (light den- red) tones to 1000 rived from GFAS (Global Fire Assimilation System) and averaged to 1 Figure 2. et al., 2012). Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | are l and g 14 wet season (1 - (b) 1 Dec

); where b + a ( / ) l + and (b) season and wet ( g ( = are the numbers of species in site 1 terra firme forest upon fluvial terrace, 30 Nov)

b = and 15 June - a 11693 11694

hourly wind speedaverageshourly of measured direction 81 mat and - seasonally flooded black-water forest (igapó). dry season (15 June–30 November) and = based on half based (a) June) for period the 2014. from 2012 to 23 July a.g.l. 18 Oct Wind roses for (a) dry season dry ( Wind 5: for (a) roses Figure

terra firme forest upon plateau, Terr = 0.0

0.6 0.4 0.2 0.8 1.0

Wind roses for

SMI (species turnover) (species SMI Species turnover of the four inventoried forest types at the ATTO site. Turnover is campinarana, and IG = Figure 5. Camp gained and lost speciesand from site 2. site TF 1 to site 2; December–14 June) basedat on 81 ma.g.l. half-hourly for averages the of period from wind 18 speed October 2012 and to direction 23 July measured 2014. Figure 4. expressed as Shmida and Wilson’s (1985) index: SMI Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | dry season 2012 2013 2014 ● (b) Dec ● Nov ●

Oct ● Sep ● Manaus 1961−1990 Aug ● Jul Month wet season (March 2014) and ● Jun

(a) 11696 11695 ● May ● Apr ● (September 2013). Contour 0.4 m, 2013). at 1.5 from plots(September m,measurements 4 m, interpolate 55 m, 81 m.12 m, 73 m, 26 m, and 36 m, 40 m, Mar ● Figure 6: Diurnal profiles of temperature for a) wet season 2014) (March and season dry b) Feb

●

Jan

100 50 0 350 300 250 200 150 Diurnal profiles of temperature for [mm] Precipitation Monthly sums of precipitation at the ATTO site for the years 2012 to 2014. For com- Figure 7. parison the data from theperiod Manaus (1961–1990)) INMET-station (www.inmet.gov.br are of shown. the standard reference Figure 6. (September 2013). Contour plots interpolate55, from 73, measurements and at 81 m. 0.4, 1.5, 4, 12, 26, 36, 40, Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | /3 -1/3 1 ), for the ATTO site from ) 10 100 10 100 ζ ), for the ATTO site from ( ζ v ( 3ζ θ w φ − φ 25(1 2(1 + 9.5|ζ|) . 1 ζ ζ − − 11698 11697 0.001 0.01 0.1 1 1 0.001 0.01 0.1 1

10 1

0.1

100 10

w 0.1 (ζ) ϕ θv (ζ) The dimensionless SD function for vertical velocity, ϕ The dimensionless SD function for virtual temperature, measurements at 39.5 m. Figure 9. measurements at 39.5 m. Figure 8. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | ), from its ζ ( a φ -1/3 ), for the ATTO site from ζ ( c φ 2(1 + 9.5|ζ|) ζ concentration, 2 − 11700 11699 , respectively. c , and q , v θ 0.001 0.01 0.1 1 10 100 1 10 0.1

100

1000 c (ζ) ϕ From top to bottom, the departure of the dimensionless SD function, The dimensionless SD function for CO Figure 11. surface-layer behavior for Figure 10. measurements at 39.5 m. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 1000 100 ] 10 time scale [s 11702 11701 Mean TKE spectra 1 80 m 42 m 23 m fluxes. 2

0.1

3 3 5e−0 2e−0 e0 5e−04 2e−04 e0 5e−02 2e−02

Upper panels: Temporal evolution of the three wind components for the night of 27 Mean multi-resolution TKE spectra at the three observation levels. ] s [ TKE m S

2 2 − Figure 13. Figure 12. April 2012 at eacheddy of covariance the CO ATTO observation levels. The lower panel shows the corresponding Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper |

)

◦

] [

m s m m 43 and m 80 between difference Wind

1 − . . . . 2.0 1.5 1.0 0.5 0.0 Schematic with (b)

ects. ff erence between the 80 and 42 m levels ff

0.003 0.002 0.002

surrounding the ATTO site in the Uatumã Sus- 0.001 0.001 surrounding the the site surrounding in SuATTO s- Uatumã the 2 2 Time [h] 11704 11703

4 May 2012, 42 m 2012, 4 May ffects.

; the black dots indicate GW events induced by terrain undulations 0.003

0.001 (a)

0.005

0.004 0.004 0.002 0.002 0.001 0.001 5: (a) Area of approximately 900 km 02468 tainable Development Reserve. The The 5°, 10°,axes (0°, represent Development Reserve. directions the 15°, ..., tainable ATTO the from 175°, 180°) tower. Color scale represents terrain elevation in meters above sea level. (b) Schematic with axes corresponding to (a); the black dots indicate the by terrain undulations points GW and represent induced GWgray events events terrain by e not induced

02468

100.0 −1.0 0101000 100 10 1 Area of approximately 900 km Figure 1

Upper panel: Multi-resolution 42 m vertical velocity spectra for the night of 4

] [m w

s

] [ T 1 s scale ime − and the gray points represent GW events not induced by terrain e from the ATTO tower.axes Color corresponding scale to represents terrain elevation in m a.s.l. Figure 15. (a) tainable Development Reserve. The axes represent the directions (0, 5, 10, 15, . . . , 175, 180 (red line, scale at thelevel right for side). the Lower same panel: night. temporal evolution of vertical velocity at the 42 m Figure 14. May 2012 (colors and contours), and mean wind di Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 60 u w T q 50 , recorded at heights of 42 and 81 m q ] [s , and T , 40 u , w 11705 11706 Temporal scale computed from the measurements in January 2013. Time is 2 30 20

Diurnal cycle of CO

Coherent structures time scale of 2.0 1.0 1.8 1.6 1.4 1.2 2.6 2.4 2.2 z/h above the ATTO site. Figure 17. given in UT, withof the local first sunrise 12 (10:00 h UT)show repeated the and heights for sunset of clarity. (22:00 the UT), The 5 respectively. white inlets. Black vertical dashed lines horizontal lines indicate the times Figure 16. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | measurements 4 11708 11707 (computed by pooling all available CH 4 Same as Fig. 17, but for CO (computed by pooling all available measurements until Same as Fig. 17, but for CH Figure 19. the end of 2014). Figure 18. until the end of 2014). Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | at the 2 4 m 38 m 79 m 07 2014 and CO recorded at the lower- 4 May 07 May 2012 2013 11710 11709 30 Apr 30 Apr 2012 2012 MAMJJASONDJFMAMJJASONDJFMAMJJASOND

250 200 150 100

] [

ppb

1900 1800 CO 2200 2100 2000

Examples of sporadic concurrent increases in CH

Statistics of monthly daytime (17:00–20:00 UT) 30 min measurements of CO

] [

4 410 400 390 380 430 420

ppb CH

] [ 2 ppm CO Figure 21. 80 m walk-up tower. Shownmeasurements. are The whisker white plots line indicatinglevel, in min/max blue: the 79 and m box quartiles level. indicates of the the median. monthly Brown: 4 m level, green: 38 m most (4 m) inlet in 2012. Figure 20. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | and 4 and CO 4 D , CH 2 N O S ● ● ● ● ● ● ● ● ● D D D ● ● ● A ● ● ● ● ● ● ● ● ● N N N ● ● ● J ● ● ● ● ● ● ● ● ● O O O 2014 2014 ● ● ● ● ● ● J ● ● ● ■ ■ ■ S S S ● ● ● ● ● ● ● ● ● ● ● ● A A A ■ ■ ■ ● ● ● M ● ● ● ● ● ● J J J ● ● ● ■ ■ ■ ● ● ● A 2014 2014 2014 ● ● ● ● ● ● J J J ● ● ● ■ ■ ■ ● ● ● ● ● ● ● ● ● M ● ● ● ■ ■ ■ M M M ● ● ● ● ● ● ● ● ● ● ● ● A A A ■ ■ ■ ● ● ● F ● ● ● ● ● ● ● ● ● ■ ■ ■ M M M ● ● ● J ● ● ● ● ● ● ● ● ● ■ ■ ■ F F F ● ● ● ● ● ● ● ● ● D J J J ● ● ● ■ ■ ■ ● ● ● ● ● ● ● ● ● ● ● ● ■ ■ ■ D D D ● ● ● N ● ● ● ● ● ● ● ● ● ■ ■ ■ N N N ● ● ● O ● ● ● ● ● ● ● ■ ■ ■ ● ● O O O S ● ● ● ● ● ● ● ● ● ■ ■ ■ S S S ● ● ● ● ● ● ● ● ● ● ● ● A A A ● ● ● A ● ● ● ● ● ● J J J ● ● ● ■ ■ ■ ● ● ● 2013 2013 J ● ● ● ● ● ● J J J ● ● ● ■ ■ ■ ● ● ● 2013 2013 2013 J ● ● ● ● ● ● ● ■ ■ ■ M M M ● ● ● ● ● A A A ■ ■ ■ M ● ● ● ■ ■ ■ M M M 11712 11711 A ● ● ● ■ ■ ■ F F F M J J J ● ● ● ■ ■ ■ ● ● F ● ● ● ■ ■ ■ D D D ● ● ● ● ● ● ■ ■ ■ N N N ● J ● ● ● ■ ■ ■ O O O D ● ● ● ■ ■ ■ S S S ● ● ● ● N ● ● ● ■ ■ ■ A A A ● ● ● ● ● ● J J J ● ● ● ■ ■ ■ ● ● O ● ● ● ● J J J ● ● ● ■ ■ ■ ● ● S 2012 2012 2012 ● ● ● ● ● ● ● ● ● ■ ■ ■ ● ● ● M M M ● ● ● ● ● ● A ● ● ● ■ ■ ■ A A A ● ● ● ● ● ● ● ● ● 2012 2012 ● ● ● ■ ■ ■ J ● ● ● M M M ● ● ● ■ ■ ■ F F F J J J J ● ● ● ■ ■ ■ M 80 60 40

120 100 395 390 180 160 140 400

] [ ] [

A 2

ppb CO ppm

CO 1850 1800 1750 1900

] [ 4 ppb MAMJJASONDJFMAMJJASONDJFMAMJJASOND CH M

50

200 150 100

] [

ppb

CO Statistics of monthly daytime (17:00–20:00 UT) 30 min measurements of CH Monthly averaged daytime (17:00–20:00 UT) measurements of CO

1860 1840 1820 1800 1900 1880 4 ] [ ppb CH at the 79 mmonthly level averaged of concentration the measurements ATTOare from tower preliminary; Ascension (blue Dlugokencky Island et line, (brown; al.,Carpenter SD 2014; data et indicated Novelli al., for and by 2010, 2014 Masarie, updated). shading) 2014) in and Cape comparison Verde with (green: Figure 23. CO at the 79and m quartiles level of of the the monthly 80 measurements. m The walk-up white line tower. in Shown the are box whisker indicates plots the median. indicating min/max Figure 22. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper |

Net Radiation Total OH reactivity -2 -1 [Wm ] [s ] 400 200 0 60 50 40 30 20 10 0 600 erent heights (0.05, ff 21:00 00:00 20 Nov 2012 isoprene OH reactivity), which 1 18:00 − 2.46 s 15:00 = 12:00 ] 12:00 11713 11714 Date and time [LT] 79.3 m Time of the day [LT 09:00 00:00 19 Nov 2012 24 m 06:00 0.05 m 03:00 12:00 18 Nov 2012 5 0

15 10 25 20 Profiles of isoprene derived from measurements at three di

5 0 Isoprene and total OH reactivity measurements during November 2012 at the high-

00:00 Isoprene [ppb] Isoprene 15 10 35 30 25 20 20

Isoprene [ppb] Isoprene Temperature [°C] Temperature est point above thewere canopy available (79 (about m), 4 binned days).contribution as The to 60 isoprene min the mixing total medians ratio OH for reactivity scale all (1 (left ppb periods axis) isoprene when was both set data to match its 24 m, and 79.3 m)from below, dry within, to wet and season). above the canopy in November 2012 (transition period Figure 25. is presented on thesured right at axis. 81 The m) and upper the panel net shows radiation. the diel variation of temperature (mea- Figure 24.

Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper |

3

[ppb] O 12 10 8 6 4 2 0 wet season Local time (UTC -4) cients and particle number concen- 0.05 m 0.5 m 4 m 12 m 24 m 38.3 m 53 m 79.3 ffi 20:00 00:00 04:00 08:00 12:00 16:00 20:00 11716 11715 mixing ratios measured on the walk-up tower during the 3 dry season Local time (UTC -4) 80 nm). > 8 6 4 2 0 Time series of scattering and absorption coe

20:00 00:00 04:00 08:00 12:00 16:00 20:00 Mean diurnal profiles of O

12 10

3

[ppb] O Figure 27. tration (diameter Figure 26. dry season (left panel,February 15 to August 3 March to 2014). 14 September 2013) and the wet season (right panel, 1 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , = 3 − cm . 3 3 − Total, dry N cm , 3 3 0.5 µm − = 7.5 µm , wet µ 967 cm = = sub- V ; 3 Total, dry − Acc, dry V , N 3 , − 3 size distributions from the SMPS − 282 cm cm 3 = (b) 395 cm . Integrated number and volume concentra- 3.5 µm = 3 Total, wet − = N cm , 3 3 Ait, dry , dry 11717 11718 − µ N and volume super- (a) 2.0 µm V 130 cm , = 3 = − cm 3 Total, wet Acc, wet V , N 3 , − 3 4.0 µm − = cm 3 , dry µ 141 cm sub- = 1.5 µm Median particle number V Intercomparison of the median particle number size distributions from the SMPS, = ; 3 − Ait, wet , wet µ N super- and OPS instruments,(solid representative lines) for conditions seasons.ering during Plotted 7 day the data periodsconditions. wet sets Integrated for (dashed comprise number lines) wetriod: and continuous and (06–13 volume dry SMPS May concentrations 2014) and for and OPS the dry selected data (13–20 wet cov- season September pe- 2014) season tions for the selected dry season period: Figure 29. V 1398 cm OPS, WRAS, and UHSAS instruments.line Instruments during were clean operated rainy-season for conditions 6 h (26 using January the 2015). same inlet Figure 28. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | = = , long µ Ait, long N super- V , 3 − cm 3 2.3 µm = , long µ size distributions from the SMPS and sub- V ; (b) 3 − size distributions of the total and fluorescent (b) 11720 11719 409 cm = . and volume 3 − (a) cm 3 Total, long and volume N , (a) 3 − 15.0 µm = 308 cm = Total, long V , 3 − Average number Median particle number Acc, long N cm , 3 3 − Figure 31. aerosol particles measured by WIBS. Orange lines refer to the size-resolved fraction of FBAP. Figure 30. OPS instruments, showing thewith contrast long-range between transport pristine influence wet (i.e.,Wet season Saharan season conditions dust, number African and and biomass episodes volumesize burning, size and spectrum spectra sea are is salt). taken averaged fromgrated Fig. from number 29. three and The selected long-range volume transport episodes concentrations in for February the and long-range March transport 2014. episodes: Inte- 80 cm 12.7 µm Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper |

aerosols col- Si 39% 2.5 30 Mar

Al 9% 2% 4% ] 12% -3 20 Mar 5%

Ti 11722 11721 3% 78% Total=0.83 [µg m Total=0.83 [µg Date, 2015

10 Mar 6% Mg

S organics sulfate nitrate ammonium chloride 18%

1.5 1.0 0.5 0.0 3.0 2.5 2.0

Mass concentration [µg m [µg concentration Mass

] Average bulk elemental concentrations (in weight-percent) of PM Time series of aerosol concentration and average chemical speciation at the ATTO -3 Fe 25% lected at 80 m height between 7 March and 21 April 2012. Figure 33. Figure 32. site, measured by ACSM during the early wet season from 1 to 31 March 2015. Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Carbon Carbon (a) (b) C) functional = C) and keto (O = 11724 11723 NEXAFS spectra showing high abundance of pi- (C STXM images and elemental maps with corresponding NEXAFS spectra of aerosol (c) Figure 34. particles collected at thepost-edge ATTO image site (293 eV) during ofticles a a with period characteristic cores with region (black anthropogenic showing arrows) pollution. internally and mixed coatings droplet-like of par- variable thickness (green boxes). elemental map (pre-edge 280 eV,material. post-edge 293 eV) showing thegroups distribution in of cores. Coating carbonaceous reveals highsignals abundance for of keto carboxylic acid and groups pi (CCOH) groups. and weaker Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 30 SEM images of STXM elemental (a) (c–f) 26 : primary biological aerosol (b) 22 18 14 11726 11725 Date (November 2012) 10 Sesquiterpene Ox. Prod. Monoterpene Ox. Prod. STXM carbon post-edge image (293 eV) and 06 (b) 04 0

80 60 40 20

100 160 140 120

] Concentration [ng m [ng Concentration Concentration of monoterpene and sesquiterpene oxidation products in ambient Microscopic images of aerosol particles during rainy season. −3 Figure 36. aerosol collected in November 2012 over the Amazon rain forest. Figure 35. representative region. maps of same region.particles The (region particle i), types droplet-like are SOAgion indicated particles iii). in (region panel ii), and potassium-rich biogenic salts (re-