Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , 3 Crutzen Chemistry ´ e Libre de and HCOOH, and Physics Discussions Atmospheric 3 , S. Turquety 1 and ), but uncertainties remain 3 , V. Duflot 1 2011 , ) and references therein). Many labora- ), is an excellent tool for observing and ect air quality in populated regions of the ff 2009 Akagi et al. , D. Hurtmans 2009 ( 31562 31561 ; , 1,2 2001 ) and 0.9–3.9 Tg (HCOOH). For NH , 3 ´ e Versailles St.-Quentin; CNRS/INSU, LATMOS-IPSL, 1 ` ) times higher than typical background values. The temporal ere, Chimie Quantique et Photophysique, Universit 3 , C. Clerbaux Clerbaux et al. 1 Langmann et al. ) and formic acid (HCOOH) total columns are presented for the 3 ). Boreal forest fires contribute significantly to these emissions and and HCOOH enhancement ratios relative to CO are presented. Strong 3 1990 , Andreae and Merlet , L. Clarisse , and P.-F. Coheur 1 1 The polar orbiting Infrared Atmospheric Sounding Interferometer (IASI), which mea- 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. UPMC Univ. Paris 06; CNRS/INSU, LMD-IPSL, Paris, Spectroscopie de l’Atmosph UPMC Univ. Paris 06; Universit sures globally the Earth’slow outgoing infrared instrumental radiation noise at ( a high spectral resolution and and Andreae are also important asNorthern they Hemisphere can ( severelytory, a field and aircraft studiesfire have plumes been conducted ( todue characterize to the composition the of lackfor of the measurements total over emission larger of areas reactive or species. periods; this is particularly true extratropical forest fires. 1 Introduction Biomass burning is a major source of atmospheric trace gases and aerosols ( year 2010. Maximum total columnsHCOOH) have and been 200 observed (for reaching NH overevolution of 40 NH (for CO and evidence of secondary formation of HCOOHing is found, 10 with times enhancement ratios reported exceed- masses emission for ratios the in period19–33 fresh July–August Tg 2010 plumes. (CO), over We the 0.7–2.6 estimate Tgthese center the quantities (NH of are total Western comparable emitted ; to they what is are emitted in the course of a whole year by all In July 2010, severalduring hundred its forest hottest and summervations of on fires the record. broke Infrared Atmospheric out Here,(CO), Sounding across ammonia we Interferometer (NH Central analyze (IASI). Carbon Russia these monoxide wildfires using obser- Abstract Paris, France 3 Received: 25 October 2012 – Accepted: 23Correspondence November to: 2012 Y. – R’Honi Published: ([email protected]) 7 December 2012 Published by Copernicus Publications on behalf of the European Geosciences Union. Y. Ngadi 1 Bruxelles (U.L.B.), Brussels, Belgium 2 Exceptional emissions of NH Atmos. Chem. Phys. Discuss., 12, 31561–31584,www.atmos-chem-phys-discuss.net/12/31561/2012/ 2012 doi:10.5194/acpd-12-31561-2012 © Author(s) 2012. CC Attribution 3.0 License. HCOOH in the 2010 RussianY. wildfires R’Honi 5 20 25 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , , – ). ). ). ◦ 2004 2012 2011 , , and CO , Turquety ) and fire Yurganov 3 ). The un- ; Shvidenko ; ); this is 400 ). 2003 Fokeeva et al. 2012 , 2009 , as well as the 2011 ; 1 , , , 2011 b ). The majority is − 2012 , Krol et al. , , ; ). Note that only the 2011 Stavrakou et al. European Commission, , ; 2011a ( 2011 2011 , , 1 , and HCOOH fire emissions − Wooster and Zhang Krol et al. 3 2011 ect the presented results are Witte et al. ; Coheur et al. , Golitsyn et al. ff Kasischke et al. ; Konovalov et al. C usually observed in the summer ◦ 2012 , 2011 and HCOOH total column maximums , Elansky et al. Razavi et al. 3 Stavrakou et al. Yurganov et al. Paulot et al. ( 1 ), with application of tabulated average values − ) and a retrieval scheme based on brightness 31564 31563 ) reported anomalously high temperatures (35– Huijnen et al. 2005 2012 ; , , and HCOOH. IASI CO observations from these fires ). Its potential to monitor CO from vegetation burn- 2011 3 ( ) and formaldehyde (HCHO) have been reported, using 3 2012 Zvyaginstev et al. , ; 2011 and HCOOH relative to CO. In Sect. 4, we calculate the , 3 ecting the air quality ( 2011 ff , Wooster et al. Witte et al. E. Section 3 presents the calculation and temporal evolution of the ), ozone (O ◦ Hurtmans et al. 2 and HCOOH are retrieved only when enough spectral information is erences (BTDs) for HCOOH ( 3 ff –150 Clarisse et al. ◦ Chubarova et al. ; ), severely a ; 2009 Konovalov et al. 2011 2011 , or volatile organic compounds, have in contrast not been exploited much. Such is the most important base in the atmosphere and is released primarily by agri- ; ). , , C, compared to average temperatures of 15–20 N and 30 3 3 ◦ ◦ During the summer of 2010, Central endured the driest and hottest Formic acid is an important volatile organic compound in the atmosphere; but un- In the next section we present the CO, NH measurements from a varietyet of al. satellite sounders ( lands, fields and urbanized areas acrosset a al. massive region around Moscow2011 ( usual magnitude of the eventtive was revealed power, for which instance reached by 19 high 000times values MW more of close than the to fire what Moscow radia- Along is ( this, observed large on emissions averagetrogen of in oxides aerosols Russia (NO and ( trace gases such as CO, tropospheric ni- July ever recorded. 41 season) and low relative humidityradiosonde measurements (9–25 %) in from Western Russia. mid–Junetiated The to hundreds intense mid–August of heat 2010, wildfires and from in wave European ini- Russia and burned forests, grasslands, crop- retrieval software ( radiation power (e.g. Here we include it asand well for for completeness, the as calculation anfrom of opportunity the to enhancement FORLI test ratios. (Fast-Optimal our Estimation We methodology Retrievals use on total Layers columns for IASI) of near-real-time NH of emission factors. Here wein study the simultaneous 2010 CO, Russian NH fires.case It is study the is first undertaken time forhave that NH such been a reported large spatial in and temporal two scale recent studies ( certainties in its global budget remain large ( 75 enhancement ratios of NH total masses and thetotal extra emitted burdens masses due over to the entire fires,the burning the related period. fluxes measurement These in issues uncertainties of Tgdaybriefly and surface discussed sensitivity, how in they Sect. a 5. In Sect. 6 we present our conclusions. ing has frequently been used.NH Measurements of other firemeasurements emission can products, directly improve such our as currently knowledge of rely fire on emissions the and remote fluxes. sensing These of fire counts (e.g. temperature di daytime data, which areIn addition, more NH sensitive toavailable (see surface Sect. concentrations, 5). have been used. observed within aand 2 the month mean period total (1 columns July for to these 1 species September) for in the the year summer 2010 of over the 2010, area 40 et al. analyzing trace gas emissions from strong fire events ( photochemically produced from non-methane hydrocarbons. Itin is the also atmosphere released from directly (primary) terrestrial emissions vegetation account and for 1–4 biomass Tgyr burning,NH for which the total culture (76 %), natural sourcesaccount (19 for %) 4 and % fossilJoint of fuel Research the burning Centre (5 total (JRC)/Netherlands %).2011 emissions Environmental Natural Assessment totaling fires Agency only 5–15 Tgyr (PBL) 5 5 15 10 10 25 15 20 20 25 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | – ). ): ◦ (1) over Witte which 2011 X 2000 ( ). Simi- ), 3 Delmas , ). When N to 30 ) and plant Koppmann ◦ 3 ; 2012 2011 ( 2007 , –75 , ◦ 1988 , erent source types, ff ). A related parameter Yurganov et al. and HCOOH. These can Xiao et al. 2011 3 ( Goode and Yokelson Yurganov et al. Parrington et al. Andreae et al. Akagi et al. and HCOOH related to thermal contrast 3 ) and 31565 31566 ) which reported mean values between 2 and 4 and HCOOH from March to the start of the fires , which is the ratio of emitted molecules of 2001 3 ( N for NH and HCOOH are shown in Fig. 1 over Europe and X ◦ 3 2012 ( ) and in laboratories ( , from 27 July (corresponding to the first IASI observation ◦ 1999 , ). Emission factors are measured both in situ (e.g. ( 0.5 ambient × . In fresh plumes, the emission ratio can be estimated from the ambient ] erent areas around Moscow. The higher than average CO total ◦ X ff X 2009 [ M [CO] erences in lifetime (see Sect. 4), but also by the fact that we have / , ff − − Mielonen et al. in di CO Andreae and Merlet 2 M − smoke smoke and HCOOH which represent 40 times for CO and HCOOH and 200 times Yokelson et al. ] erence between the spatial extents of CO, NH ) and ). Large compilations of emission factors, grouped in di ; 3 ff X [ [CO] Reid et al. higher than typical background values. These maximum emissions are followed 2011 3 2005 )( = 1995 ( 1 E, is the same area as the one considered in the study of , moleccm , − ◦ X 18 As the plume ages, the enhancement ratios will typically decrease for species with Very high total columns were observed during the event for the three species. Fig- CO ∆ ∆ are due to the usual seasonality of that species, maybe intensified in springtime by the 10 columns observed above Central Russia between January and June 2010 (Fig. 2b) transport of fire plumes from outside the studied region ( et al. 3 Enhancement ratios Fires emit tracesource gases material. in A amounts usefulemission parameter that factor, to depend which quantify on is tracegkg gas the the emissions specific amount fromet of fire fires al. emitted conditions is the species and per amount ofcan dry be found fuel in (in larly, the progressive increase incan NH be explained with the increasegrowth in (for spring HCOOH). of As agricultural explained activities above,tumn the (for and NH lack of winter retrieved is HCOOHfor due columns the in to conditional au- too retrievals. low thermal contrasts, not exceeding the 5 K threshold a lot of observations are available, the enhancement ratios can be calculated for each for CO, NH for NH by a rapid decrease inground the values after concentrations 20 of August. theseis This species the decrease and shortest-lived is return species especially of to(Fig. pronounced the typical 2b), for three. back- NH are The mean inet CO good al. total agreement columns, with presented here recent studies of molar masses ratio of concentrations, the so-called enhancement ratio ( a lifetime shorter than CO.insight The time into evolution of the the chemical enhancement ratio loss therefore processes gives within the plume ( a two months period whichcorresponding includes to the the fires red (1year July box 2010 to in 1 covering Fig. September 1; theemissions 2010) Fig. at same in the 2b the area. end area shows of From thecisely July Fig. on which mean 2a corresponds July total to 27) one columns the reaching sees beginning for a of the maximum a the emission significant fires on (more increase 2, pre- 10 of and 15 August, respectively is the emission ratio ofthe a number trace of gas emitted molecules ofsion a ratios target can species such be as calculated CO, from used hereafter. emission Emis- factors by multiplying with the ratio of the be explained by di a more limited sensitivity above(see 55 Sect. 5). Note150 also that theThis red choice box in was Fig. madeearlier 1, intentionally study. extending to from facilitate 40 the comparison of ourure results 2a to shows that the temporal evolution of the retrieved total column maximums during Average total columns of CO,Asia NH in grid cells ofof 0.5 the fire plumes)is to some 27 August di (a few days after the end of the fires) of 2010. There 2 Distributions and time series of total columns 5 5 25 10 25 20 15 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 3 is (2) S total 3 3 columns Yokelson 3 . For NH ). 2 ) and cm ). In contrast, the 2009 17 2000 , ( ). A likely explanation 10 2011 × is the Avogadro number , 2011 a ( N ) and other types of vegetation, enhancement ratios start around and 0.021 for HCOOH. Enhance- Coheur et al. 3 is the mean column retrieved from 3 and HCOOH vs CO on 5 August. 2011 Akagi et al. X , 3 C Akagi et al. have been calculated here as follows: CO ( ∆ ), ). In a first step we estimate the daily total X 1 − Goode and Yokelson , see Fig. 2b), vs 2 − X 2011 31567 31568 cients around 0.75) are indicative of the com- ( ∆ E) and this is justified by the fact that FORLI-NH ffi ◦ (in gmol of species –90 Konovalov et al. ◦ X X TM Yurganov et al. N and 30 ],[CO]), while an average enhancement ratio can be estimated ◦ ), likely correspond to aged air masses. For this day of 5 August, X 2 ) in Fig. 3a, which are associated with rather high columns of CO − –75 2 ◦ − S X a ) describe this process and report enhancement ratios in downwind plumes C is the molar mass of N X moleccm X and 0.70 Tg for HCOOH. M moleccm cult to compare the results to a single emission ratio. We find, however, that for 18 M represents a defined surface area. For CO and HCOOH the latter corresponds 3 2007 ffi ( = 16 the range of values measured from IASI (0.010–0.055) is consistent with the val- S X 3 10 4 10 After having calculated the daily total masses over the area of interest it is possible to As the 2010 Russian fires are associated with the burning of both peat lands (ac- Enhancement ratios for the Russian fires are shown in Fig. 3 over the area de- < > the minimum of theare total plotted masses in observed the in 10 middle day panel intervals. in The Fig. resulting 4. burdens Maximum burdens are calculated at around for this discrepancy is(e.g. rapid secondary Yokelson et production al., of 2009). formic For acid within instance; the fire plume daily evolution of thesmoothed). total The masses total masses for reach in thefor mid year NH August maximums 2010 of (in 36.1 Tg black for CO, daily 0.06 Tg values andestimate in the red total emissions by makingproach some similar extra to assumptions. that Here of wemass follow an due ap- to thevalues. The fires background (the values so-called (Fig. 4 burdens) left by panel subtracting in total blue) were mass obtained background by smoothing between 0.023 and 0.029, whichratios are found in here. much A better more agreement general with interpretation the of enhancement the enhancement ratios measured and to the red rectangle identified ina Fig. smaller area 1 (40 and is estimatedis at a 2.75 conditional retrieval method,this as species discussed previously, prevents and its that the long-range short transport. lifetime Figure of 4 shows, on the left panel, the 4 Total mass Daily observed total masses TM where IASI daytime observations (in molec cm transport patterns: the buildupular of mean CO that during the the realratios. emission entire ratios burning are period still could higher in than partic- our reported enhancement calculated values vary betweenmagnitude larger 0.010 than and emission ratios 0.030 values in for HCOOH, and are one orderet of al. by IASI is, however, hampered by the continuous emission, production and complex NH ues reported in thefor literature, boreal which average forest 0.033 fires for and extratropical forest 0.097 fires, for 0.035 peat lands ( it is di from the slope of the linear regression measurement pair ([ pointing to a decreasepronounced in variations of fire the activity enhancement and ratio are a found return for HCOOH. counting to for background 30 % CO of columns. emitted CO Less ( mon emission source for the( three species. Note( that the series ofthe low calculated enhancement NH ratios are 0.032ment for ratios NH are calculated similarlyfrom 27 for July each to day 24 and August0.015 is the on shown corresponding in the time Fig. 27 3b. evolution July Forcolumns NH and are reach a largest maximum (Fig. of 0.055 2). on After the that, 10 August the when enhancement NH ratio decreases gradually, fined above. Figureratio, 3a the shows scatter anThe plots high example of correlations of (correlation total coe the columns calculation of of NH the enhancement 5 5 25 20 10 15 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 1 1 ). − − er- (3) ff . This ). The ) (19– 2001 erence X , ). Di ff 2012 2011 ( ( 2011 ective lifetime ( ff erent lifetimes. ff is time between t , Aneja et al. i ) who use direct CO ; Krol et al. 2011 1998 , 0.04–0.07–0.15 Tgday ( 1 Fokeeva et al. , − Fokeeva et al. ) and obtained using inverse ) and set estimated from the di 2012 ( ff and HCOOH, this is comparable to ective lifetime of the species ff 3 2011 ( culty in estimating total emitted masses Asman et al. . Finally, total emissions were estimated ). Fokeeva et al. ffi ; ff and HCOOH respectively, with the larger e ) (26.2 Tg) and 3 τ and HCOOH maximum values reported here is the e Krol et al. 2011 3 31570 31569 ff 1994 ) and ): , e , especially not in such an extraordinary event, , 2011 τ 3 ( 2011 1999 ( , ). It should be noted though that for HCOOH the values and 0.35 Tg for HCOOH. Note that a 10 Tg of CO bur- Yurganov et al. for CO, NH ), the daily fluxes for CO have been estimated using two 3 ) represent primary emissions only. 1 − 2001 Jacob , ff 2011 ) e ( of the species. Following estimates of the CO e ff 2001 e Stavrakou et al. ( ) and that the NH ff t/τ ; e − t/τ Yurganov et al. τ − e i e 2011 B Yurganov et al. 2004 , are respectively the flux and the burden on day − , Dentener and Crutzen − i namely 7 and 15 days. As we do not have accurate knowledge of the (1 1 B ff + ff i ) and 0.9–3.9 Tg (HCOOH). For NH e e 3 τ B τ and Yurganov et al. = i ) ective lifetime E Andreae and Merlet X ff ( , we use lifetimes of 6, 12 and 24 h as its lifetime ranges typically from a couple of 1 3 ective lifetime of HCOOH and NH Andreae and Merlet There is a large scatter in the data, both for the maximum daily emissions (1.2– Several estimates of total emitted CO have been reported in the literature for the From the burdens we can calculate emission fluxes assuming a simple box model + i ff Galloway et al. Konovalov et al. wide scatter in the datafrom is satellite evidence data. of the For di CO our approach gives a rather large but realistic range of 26 Tg) agree wellstudies with use similar our approaches. estimates Theirconcentrations (19–33 adjusted are Tg). values, about This with 40 enhancedwell % is boundary with higher. not layer The the surprising total valuesmodeling as 20–25 emissions of Tg all reported IASI given three here CO in ary also data. layer agree As using they averagingovercorrection kernels take in this into the papers is account of somehow IASI’sences surprising sensitivity and but potential to points sources the of to bound- errors a are possible discussed in detail in between satellite and ground based measurements.dard” For and these “adjusted” studies indicate the whether labels adjustments “stan- were made. 2.4 Tg) and thesurements total found emitted in CO (10–40 Tg). The standard estimates from CO mea- measurements, allowance is madeto for boundary the layer limited concentrations by sensitivity adding of an infrared o instruments ( 2010 Russian fires, andthe these one have hand been estimatesIASI, derived summarized AIRS from in and CO Table MOPITT) measurements 1.on possibly (from the These coupled the other with include hand infrared an on estimatesIn sounders atmospheric derived the transport from studies model, MODIS of and fire radiative power measurements. and 0.07–0.11–0.19 Tgday values logically for thefrom smaller these values fluxes between of 2.6 15 Tg July (NH and 31what August is 2010 normally and are emitted 19–33 in Tg the (CO), course 0.7– of a whole year by all extratropical forest fires of these species for thesemaximum various values calculated lifetimes, this from way 29 are June 1.41–1.87 Tgday to 27 September 2010. The The right column of Fig. 4 shows the time evolution of the (smoothed) fluxes in Tgday in and first order loss terms ( values of e we calculate also forThis these approach allows species to the conservativelywith estimate fluxes the a for IASI range measurements. a of For wideestimated total HCOOH, we emissions lifetime range use of compatible of 2, 3–4 4 di daysNH and (see 10 Stavrakou days et following its al.hours global 2011 to and references days therein). ( For den represents more than 85( % of total annual anthropogenicaccount emissions alone in for that 5 region fires and ( 20 % of the total annual emissions from extratropical forests lifetime term includes chemicalconsidered area. losses, Here, but we alsoneglect assume potential losses inflow that of due all excess columns. burdens tothe The are calculation e transport thus due depends outside to exclusively on the given the in Russian fires and 10 Tg for CO, 0.04 Tg for NH E Here two observations (here one day) and 5 5 25 15 20 10 25 20 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Razavi in the case 3 and HCOOH 3 Yurganov et al. an emission ratio and HCOOH, we was conditionally 3 3 3 erence, the so-called ther- ff ), especially when there is lim- ). Daytime observations typically 2009 , 2011 , 31571 31572 ). However, the total error can be much larger ), we do not expect a consistent low bias of the ective lifetimes quite large, as to obtain a range of George et al. Razavi et al. ff (see Sect. 4). Finally, the retrieval of HCOOH relies 2012 2012 ; ( ) found large underestimates in CO total column re- 3 , ) estimate average uncertainties to be about 60 % for and HCOOH. We presented total columns (maximum and HCOOH, these are the first values reported. They 3 and the thermal contrast). While we obtain less measure- 2010 3 2011 , 3 ( 2011 an accurate error could only be obtained via validation. Note ( 3 , the enhancement ratios were shown to be in good agreement ective emission ratios using the median estimates of the total Krol et al. 3 ff ). Note that the selection criteria might lead to an underestimate of relative to CO for each day and reported their time evolution during 3 Hurtmans et al. 2010 , Clarisse et al. Fokeeva et al. Razavi et al. ) we have restricted retrieval to observations with a thermal contrast above 2011 ) and ( Retrieval errors for ammonia are larger than for CO, because of smaller signal to We can calculate e 2011 Clarisse et al. both the total column ofments NH in this way, the measurements which are retained have limited dependence on assumptions on the speciesto previous lifetimes. studies. For For CO, NH the results obtained are comparable ( trievals as compared toour ground-based total measurements mass close estimate tomodelling Moscow. approach is However, of in as excellentretrieved agreement CO columns. with a more sophisticated inverse noise ratios and largerretrieved dependence from on IASI thermal spectra, on contrast. the Here, basis of NH a firm spectral signature (which depends on and mean) from IASIof observations HCOOH for and NH 2010. Wethe have fire calculated period. enhancement For ratios NH with tabulated values of emissionorder ratios, while of for magnitude HCOOH larger. ourtion This reported of values is HCOOH are suspected in one the to plumes.found be For around both due mid-August species where to the the maximum the total enhancementculated rapid ratios columns total were are secondary masses largest. forma- In and addition, the we burdens have cal- from fires for each day, as well as fluxes using ited sensitivity to the boundary layer. As we have mentioned in Sect. 4, 6 Conclusions The fires which occurred inties Russia of during trace the gases summer andtrace 2010 aerosols gases emitted for important almost namely a quanti- CO, month. NH In this work, we focused on three et al. 5 degrees. such conditions. The algorithm doestions, however but not simulate provide to errors NH onthat individual uncertainties observa- related to limitedin sensitivity the of calculation the of boundary enhancement layer ratios. partially cancel out have a larger thermal contrastpass than night to time study observations and thesebelow are species. the 10–15 % preferred FORLI over- ( COsuch retrievals as have in on the case average of a strong retrieval fires error ( of extreme conditions as thoselocated reported in here is situ outside measurement the arethe scope boundary the of layer only this a way paper, retrieval as to error( col- assess of 30–50 it. % For for agricultural the total pollution column in has been estimated the a priori column (low smoothing error). An estimate of the error for NH the total burden and masson of conversion from NH BTDs and is also dependent on the thermal contrast. As in For HCOOH an average emission ratioenhancement of ratios 0.047 (0.020–0.030 is found, for also the higher most than active the period). observed 5 Discussion The sensitivity of IASIdepends to heavily on lower the tropospheric surface-atmospheric temperature concentrationsmal di of contrast ( CO, NH have taken the range ofreasonable possible values e for the total emissions. emissions. Assuming a total COof emission of 0.082. 26 This Tg is we obtain naturally for larger NH than the observed enhancement ratios 0.010–0.055. values, and gives confidence to our methodology. Likewise, for NH 5 5 25 25 20 15 20 10 15 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , , , 31566 , 1995. , 1998. 31566 , , 1988. 31562 and 0.9–3.9 Tg for 3 , 2001. 10.1029/2009JD013291 10.5194/acp-11-4039-2011 10.1007/BF00546762 31569 31564 ´ e) with F.R.S.-FNRS. C. Clerbaux , 1994. , 2012. 31562 10.1029/JD093iD02p01509 10.1046/j.1469-8137.1998.00180.x ce for Scientific, Technical and Cultural Af- ´ ffi e de Franc¸aise Belgique) and by the EU-FP7 31567 31569 , 31562 10.1029/2000GB001382 , 2009. 31574 31573 and HCOOH comparable to what is emitted in ` a la Recherche dans l’Industrie et dans l’Agriculture 3 31563 , 2001. 31563 , 1990. depending on the choice of reference lifetime. When 10.1007/BF00694492 1 − , 2009. 10.5194/amt-5-557-2012 ´ ees” (Communaut , 2011. 31567 , IASI has been developed and built under the responsibility of the Centre 10.5194/acp-9-6041-2009 ects during extreme fire event over Central Russia in summer 2010, Atmos. 31566 31572 ff , , ´ Etudes Spatiales (CNES, France). 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Andreae, M. O. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, a year by all extratropical forest fires. Acknowledgements. National d’ of the EUMETSAT Polar System.real The IASI time L1 data data distribution aretaken received service. within through Part the the of O3SAF EUMETCastby near the and the work supported F.R.S.-FNRS, the on by Belgian EUMETSAT. COfairs The State and benefits research Federal the from in O European the Belgium“Actions Space activities was de Agency Recherche funded under- Concert (ESA-Prodex arrangements). Financial support by the are of the orderintegrated of over 0.1 the Tg entire day firelate period to (July–August a of total 2010), emittedHCOOH. the mass For emission of all 19–33 fluxes Tg these trans- foremission. species, CO, For there 0.7–2.6 instance Tg is for this a NH is significant for contribution NH to the yearly global 5 5 20 30 10 15 25 20 25 10 15 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | , , 31570 31569 , 2003. , 2009. 31580 , 2012. 31569 , , , 31571 , HCN, NO, , 2 31564 H 31564 31567 2 , , ,C 31563 4 31564 31563 , 2012. 31564 , CH 2 , 2012. , 2012. , 2011b. , CO 3 10.1029/2003GL017859 , 2011. ˜ ao, J., Heil, A., Eskes, H. J., 10.5194/acp-9-8317-2009 10.1134/S1028334X11120014 31567 31580 , , 31566 31563 OH in 1997 Alaskan biomass burning plumes 31565 31562 3 31564 31566 31571 10.5194/acp-12-4341-2012 31576 31575 , 31570 , 2005. , 2011. 10.1016/j.jqsrt.2012.02.036 , 2012. , 2009. , 2000. 31570 , 2011a. , , 2004. 10.5194/acpd-12-28705-2012 10.1134/S000143381106003X 10.5194/acpd-11-12141-2011 31564 COOH, HCHO, and CH 3 10.1029/2000JD900287 10.5194/acpd-5-10455-2005 http://edgar.jrc.ec.europa.eu 31580 , , HCOOH, CH 10.1016/j.atmosenv.2011.07.016 10.1016/j.atmosenv.2008.09.047 10.1007/s10533-004-0370-0 10.1134/S1028334X11030020 3 ¨ oosmarty, C.: Nitrogen cycles: past, present and future, Biogeochemistry, 70, 153–226, Lehtinen, K., and Arola, A.: BiomassRussian burning wildfires aerosols observed in in summer Easterndoi: 2010 during – the part 2: remote sensing, Atmos. Environ., 47, 279–287, 31571 fire emissions and theirdoi: impact on and climate, Atmos. Environ., 43, 107116, P.: How much CODiscuss., 12, was 28705–28731, emitted doi: by the 2010 fires around Moscow?, Atmos. Chem. Phys. spheric impacts of thethe 2010 extreme Russian air wildfires: pollution episodecuss., integrating in modelling 11, the and 12141–12205, Moscow measurements megacity doi: of region, Atmos. Chem. Phys. Dis- sions, part I:pounds, and gaseous nitrogen emissions10516, containing doi: of compounds, carbon Atmos. monoxide, Chem. methane, Phys.Sedano, volatile F., Discuss., Bergamaschi, P., organic El 5, Hajj, 10455– com- M., Kaiser, J. W., Fisher, D., Yershov, V., and Muller, J.- NH by airborne Fourier transform infrared spectroscopy22166, (AFTIR), doi: J. Geophys. Res., 105, 22147– 31563 31580 Lazaro, J., Edwards, D.monoxide P., distributions Worden, from H.,remote Luo, the sensors, M., IASI/METOP Atmos. Rinsland, mission: Chem.31571 C., evaluation Phys., and 9, with 8317–8330, McMillan, other doi: W.: space-borne Carbon keeva, E. 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C., Helmig, D., 5 5 30 25 20 15 10 15 30 20 25 10 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | and HCOOH from current and 3 erent sounders (IASI, AIRS and MOPITT), adjusted erent sounders (IASI, AIRS and MOPITT), adjusted ff ff IASI-OE standard IASI-OE standard 31564 31580 31579 ) 1 − HCOOH Comment , 2011. 3 Total emitted (Tg) CO NH Max. daily emission (Tg day ) 9.7 – – MODIS, inverse modeling )) 26.2 34–40 – – – – IASI-OE, standard Estimate from 3 di )) 1.5 2.1–2.2 – – – – Estimate from 3 IASI-OE, di standard ))) 19–26 36–42 12–14 – – – – – – AIRS-MOPITT, standard AIRS-MOPITT, adjusted MODIS, inventory method )) 1.2–1.4 2.3–2.4 – – – – AIRS-MOPITT, standard AIRS-MOPITT, adjusted ) 12.2 – – MODIS, inventory method (GFASv1.0) 2011 ( 2011 2011 2011 2011 ) 20–25 – – IASI, inverse modeling ( ( ( ( 2011 2011 2011 2011 2011 ( ( ( ( ( 2012 ( 2012 ( Comparative analysis of total emissions of CO, NH 10.1134/S0001433811060168 Konovalov et al. Krol et al. Yurganov et al. Fokeeva et al. Huijnen et al. Yurganov et al. Fokeeva et al. Fokeeva et al. This study 19–33 0.7–2.6 0.9–3.9 Fokeeva et al. Fokeeva et al. Yurganov et al. Yurganov et al. This study 1.41–1.87 0.04–0.15 0.07–0.19 Lapchenko, V. A.,nikova, E. Lezina, G., E. Tarasova, O. A., A., under and the Shalygina, Milller, host I. summerdoi: E. Y.: conditions Air of pollution A., 2010, over Izv. European Milyaev, Atmos. Russia Oceans. V. and Phy., 47, A., 699–707, Popikov, A. P., Semut- previous studies of the 2010 Russian wildfires. Table 1. Zvyaginstev, A. M., Blum, O. B., Glazkova, A. A., kotelNikov, S. N., Kuznetsova, I. N., 5 - cy (2) Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | September during the have been respectively st 3 X CO o NH

vs

for one . The and ∆X ◦ July and 1 18 16 16 CO st 5 4 3 2 1 0 14 12 10 8 6 4 2 0 8 7 6 5 4 3 2 1 0 0.5 CO x 10 S x 10 x 10 total columns of species 30/8 (a) (b) X a × and HCOOH, X C ◦ N 3 X ) for 1/12 in the 2010 Russian wildfires 1 M TM − HCOOH , for the year 2010.

= 150 150 150 and 3 X 1/11 sr cm respectively were con- 20/8 2 NH 3 , TM HCOOH HCOOH CO 1/10 E for CO, NH and ◦ (W/cm and 3 6 3 − 1/9 , in grid cells of 0.5 10/8 2 NH –150 ]), while an average enhancement ratio can NH ◦ − , CO 1/8 ],[ CO and 3 10 X (Coheur et al., 2009). N, 30 8 ) for CO and NH 100 100 100 ◦ − 1

As the plume ages, the enhancement ratios will typically Enhancement ratios for the Russian fires are shown in − 1/7 E for (red) and HCOOH (blue) total column maxi- 31/7 ◦ decrease for species withtime a evolution lifetime of shorter thesight enhancement than into the ratio chemical therefore loss processes giveset within in- the al., plume 2007). (Xia enhancement When ratios a can lot be of calculatedpair observations for ([ each are measurement available, the be estimated from the slope of the linear regression ∆CO ical forest fires, 0.035peat for lands boreal (Akagi forest etvalues fires al., vary and between 2011). 0.097 0.010one In and for order 0.030 contrast, of for the magnitude HCOOH, larger calculated Akagi than and et emission al. are (2011). ratios values Ais likely in explanation rapid for secondary this discrepan productionplume of (e.g. formic Yokelson et acid al. within (2009)).Yokelson (2000) the For and fire instance; Yokelson et Goode al. and (2007) describecess this and pro report enhancement ratiostween in 0.023 downwind plumes and be- 0.029, whichwith are the in enhancement much ratios better foundterpretation agreement here. of A the more enhancement general ratioshowever, in- hampered measured by by IASI the is, continuousand complex emission, transport patterns: production the buildupentire of burning period couldemission in ratios particular are mean that stillment ratios. the higher real than our reported enhance- 4 Total Mass Daily observed total masses calculated here as follows: (blue) total column maximums between 1 –75 3 ◦ in the 2010 Russian wildfires 3 es. The 3 panels show the mean Dates of 2010 of Dates 165 170 srcm -150 . 200 205 210 215 1/6 ◦ io X 2 , - (1) e 31582 31581 − er /M da 3 und 3 CO CO HCOOH HCOOH N, 30 1/5 NH ◦ . 21/7 , which is NH on Au- and X ), likely (Wcm columns uare less than 3 10 3 2 -75 and 0.021 6 ◦ , used hereafter. 3 − − CO 3 NH 1/4 enhancement (red) and total columns CO ambient NH ] 50 50 50 vs for one month, from July 27 to August 27 of 2010. 3 3 3 ambient NH ] HCOOH HCOOH ◦ HCOOH X CO over the number of emit- [ [ 1/3 0.5 NH 11/7 NH NH − − X ×

◦ molec cm and 3 10 CO CO smoke smoke 8 ] ] 1/2 18 − HCOOH of July and reach a maxi- X [ (black), CO [ th and HCOOH total columns in moleccm 4 10 = and 3 1/7 1/1 CO the range of values measured > 3 0 X ( 18 18 18 18 16 16 16 16 19 19 19 19 17 17 17 17 CO 0.0 3 ∆ ∆ 3 columns. Less pronounced varia- , in grid cells of 0.5 NH 2 4x10 3x10 2x10 1x10 of August when Mean total column over the area 40 − CO HCOOH NH NH 3.0x10 2.5x10 2.0x10 1.5x10 8.0x10 6.0x10 4.0x10 2.0x10 8.0x10 6.0x10 4.0x10 2.0x10 CO th Temporal evolution of CO (black), NH

0 0 X TC-mean, [molec cm [molec TC-mean, X ] ] cm [molec TC-max, X 0

CO

2 - 2 - IASI morning observations of the 2010 Russian wildfires plum (b) ) in Fig. 3a, which are associated with 40 30 80 70 60 50 40 30 80 70 60 50 80 70 60 50 40 30 2 IASI morning observations of the 2010 Russian wildfires plumes. The 3 panels show − (Goode and Yokelson, 2000): ted molecules of a targetEmission species such ratios as can bemultiplying calculated from with emission the factorsIn ratio by fresh of plumes, thethe the molar ratio emission of masses ratio concentrations, can M the be so-called estimated enhancement rat from the ratio of emitted molecules of parameter is the emission ratio of a trace gas Fig. 1. in molec cm Y. R’Honi et al.: Exceptional emissions of . Enhancement ratios are calculated similarly Fig. 2. (a) mums between 1 July and 1square September less 2010. than Only retrievals 3 with 10 spectral residual root-mean- sidered. Fig. 1. the mean CO, NH month, from 27 July to 27 August 2010. for the year 2010. molec cm a. Temporal evolution of 16 HCOOH 10 As the 2010 Russian fires are associated with the burn- < Fig. 2. 2010. Only retrievals with spectral residual root-mean-sq 4 Y.R’Honietal.:Exceptionalemissionsof Konovalov et al. (2011)) anddifficult to other compare types the of results to vegetation,find, a it however, single is emission that ratio. for from W IASI (0.010–0.055)ported is in consistent the with literature, the which values average re- 0.033 for extratrop plots of total columns of correspond to aged air masses.calculated For enhancement this ratios day are of 0.032 August for 5, the ing of both peat lands (accounting for 30% of emitted Fig. 3 over theample area of defined the above. calculation of the Figure enhancement 3a ratio, shows the scatt an ex- for for each day and the27 corresponding to time evolution August from 24 July is shown in Fig. 3b. For return to background tions of the enhancement ratio are found for gust 5. The high correlations0.75) (correlation coefficients are aro indicative ofthree the common species. emission source for Note the that the series of low ratios start around 0.015 on the 27 are largest (Fig. 2).creases gradually, pointing to After a that, decrease in the fire activity enhancement an ratio de- mumof0.055onthe 10 were considered. b. Mean total column over the area 40 ( rather high columns of 195 175 185 190 180 , s 3 ort (3) and NH Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | 3 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | NH and 1 – ◦ − . This lifetime re, along with the X eff )

burden represents

eff u d t/τ to

HCOOH

− t/τ 12 CO e − -2 i -2 e (b) , calculated as the slopes of (a) B -1 − = 6 h = 12 h = 24 h 1 2 3 − = 7 days = 15 days

77.010 1 2 = 2 days = 4 days = 10 days CO 1 2 3 25.410

(1

x x +1 x ) and 0.9–3.9 Tg 22/8 -3 eff i -3 3 ound concentrations. have been reported τ B

August of 2010 of August NH the values in Andreae and Merlet

, this is comparable to CO of the species. Following estimates . The red lines are the E (see red box in figure 1). have been estimated using two val- 05 10 ◦ 3 and HCOOH relative to measurements, allowance )= relative to eff 19/8 3 X τ in the 2010 Russian wildfires -150 ( ◦ CO CO Emissions, Tg day Tg Emissions, HCOOH measurements (from the infrared kground values from the total masses. +1 = 0.75, y = 21.5 = 10 0.75, = y i

are respectively the flux and the burden on N, 30 HCOOH R = 0.73, y = 31.6 = 10 0.73, = R y ◦ R ), 0.7–2.6 Tg ( and CO i E August of 2010. Linear regressions are plotted for E for NH 3 29/6 14/7 29/7 13/8 28/8 12/9 27/9 HCOOH 16/8 -75 B HCOOH ◦ . Note that a 10 Tg of 2.0 1.5 1.0 0.5 0.0 ◦ CO th

0.20 0.15 0.10 0.05 0.00 0.15 0.12 0.09 0.06 0.03 0.00

E. The errors bars are the corresponding slopes errors. NH and effective lifetime given in Yurganov et al. (2011), ◦ maximum values reported here account alone for 8 namely 7 and 15 days. As we do not have accurate 3 and –90 and ◦ 3 is time between two observations (here one day) and ) -90 eff i NH -2 τ ◦ CO ). For 13/8 t E , NH i is the effective lifetime of the species HCOOH From the burdens we can calculate emission fluxes assum- N, 30 and HCOOH smoothed burdens in Tg from ◦ eff Several estimates of total emitted 3 for Here day HCOOH 5 and 20% offorests the fires total (Andreae annual and emissions Merlet,though 2001). from that extratropical It for should(2001) be represent noted primary emissions only. ing a simple1999): box model and first order loss terms (Jacob, τ more than 85% ofthat total region annual (Konovalov anthropogenic et emissions al., in 2011) and that the term includes chemical losses, but also lossesoutside due the to considered transp area. Here, we assume that all burden are due to the Russian fires andcess neglect columns. potential inflow of The ex- calculationthe effective thus lifetime depends exclusivelyof on the the daily fluxes for ues of knowledge of the effective lifetime of

HCOOH

what is normally emitted inextratropical the course forest of a fires whole (Gallowayet year al., by et 2011). all al., 2004; Stavrako in the literature forbeen summarized the in 2010 Table 1. Russianestimates These fires, derived include from and on these the onesounders have hand IASI, AIRS andan MOPITT) atmospheric possibly transport coupled model, with timates and derived from on MODIS thements. fire other radiative In hand power the es- studies measure- ofet Yurganov al. et (2011) al. (2011) whois and made use Fokeeva for direct the limitedboundary sensitivity layer of concentrations by infrared adding instruments an offset estimate ( from these fluxes betweenand July are 15 19–33 Tg and ( August 31 of 2010 molec cm molec 10/8 N and 30 18 in the 2010 Russian wildfires 5 ◦ –75 ◦ 6 285 290 295 280 total columns for 5 245 250 255 260 e Dates of 2010 of Dates Burdens, Tg Dates of 2010 Dates -75 31584 31583 d l- S and ◦ calculated by equation 3. ns nd the al; the blue lines are total masses representative of backgr 3 CO [CO] (10 [CO] 7/8 ents for the resulting slopes and their errors are given in the figu is the n 40 NH , ncement ratios of HCOOH 8 6 4 2 0 X 29/6 14/7 29/7 13/8 28/8 12/9 27/9 10 HCOOH , we use life- 0.4 0.3 0.2 0.1 0.0 , 0.06 Tg 3 CO

0.04 0.03 0.02 0.01 0.00

, 0.04–0.07–0.15 and 4/8 1 ), C and and 0.35 Tg NH for 3 CO 4 − 1 HCOOH 1 3 3 masses in Tg (black dots and line) over the area 40 and HCOOH total columns vs. CO total columns for 5 August − − NH 3 is a smaller area smoothed burdens in Tg from fires obtained by subtracting bac and NH NH S 1/8 and HCOOH masses in Tg (black dots and line) over the area 40 total columns vs. HCOOH 3 3 HCOOH CO

HCOOH E. The errors bars are the corresponding slopes errors. and , we use 2, 4 and 10 days follow- (in g mol NH respectively of 3 ◦ 1 . 3 3 and − and HCOOH calculated by Eq. (3). X NH 2 3 . Finally, total emissions were estimated 29/7 , 3 NH HCOOH HCOOH –90 NH eff Total Masses, Tg Total Masses, Observed Smoothed Background NH τ ◦ Temporal evolution of the enhancement ratios of NH CO HCOOH , is the Avogadro number and . For , 0.04 Tg for E for CO and HCOOH and 40 2 a ◦ and CO (b) 3 of these species for these various lifetimes, from and 0.07–0.11–0.19 Tg day cm CO 1/1 1/3 1/5 1/7 1/9 1/11 respectively, with the larger values logically for the . HCOOH 26/7 1 1 36 32 28 24 20 4 3 2 1 0 0 0.7 0.6 0.5 0.4 0.3 0.2 0.1 0.0 Scatter plot of NH 60 50 40 30 20 10 E) and this is justified by the fact that − − R 0.06 0.05 0.04 0.03 0.02 0.01 0.00

Left: total ) cm molec (10 [X] 3 17

NH

◦ –150

H O O C H O C H N

2 - 17 C 1000 0 0 0 1 x ] [CO / ] X ◦ N and 30 Left: total CO, NH ◦ -90 Middle: extra Right: Fluxes in Tg day especially not in suchalso an for these extraordinary species event, thelifetimes. we fluxes for calculate a This wide approach range of allows different to conservatively estimat times of 6, 12from and a couple 24 of hours hours toand as days Crutzen, (Asman its 1994; et lifetime al., Aneja 1998; ranges etFig. Dentener al., typically 4 2001). shows The the rightTg time column day evolution of of theJune (smoothed) fluxes 29 in tocalculated September this 27 way are of 1.41–1.87 Tg 2010. day The maximum values The red lines are the smoothed total masses in 10-days interv a range of totalsurements. emissions For compatible withing its the global IASI estimated mea- et lifetime al. of (2011) 3-4 and days references (see therein). Stavrakou For Tg day HCOOH smaller values of Fig. 4. 6 Y.R’Honietal.:Exceptionalemissionsof ◦ cient N, 30 ffi –75 270 275 265 ◦ ◦ is a conditional retrieval method, as discussed , see Fig. 2b), N 3 Fig. 4. smoothed total masses inbackground concentrations. 10-days Middle: interval; extra CO, the NH bluefires obtained lines by subtracting are background total values from masses the representative total masses. of Right: fluxes in Tgday 75 respectively of NH Fig. 3. (a) CO, calculated as the slopes40 of the linear regressions from 27 July to 24 August, in the region 2010. Linear regressions arevalues plotted for for the resulting both slopes speciescoe and as their red errors are and given blue in lines, the respectively. figure, The along with the correlation is the molar mass of 2 − X and 0.70 Tg for N and30 NH ◦ 3 M a. Scatter plot of -75 NH ◦ After having calculated the daily total masses over the latter corresponds to the red rectangleis identified estimated in at Fig. 1 2.75 a 10 represents a defined surface area. For previously, and that the short lifetime of this species prev the linear regressions from July 27 to August 24, in the regio where mean column retrieved frommolec IASI cm daytime observations (in (40 FORLI- its long-range transport.the Figure daily 4 evolution shows, of on theblack the total daily left masses values panel, for and thereach in in year red mid 2010 August smoothed). (in maximums of The 36.1 total Tg for masses for area of interest it is possible to estimate the total emissio by making some extraproach assumptions. similar Here to we that followstep an of we ap- Yurganov estimate et the al.so-called burdens) (2011). daily by subtracting total total In mass mass a background due va first to the fires (the in the middle panel inlated at Fig. around 4. 10 Maximum Tg for burdens are calcu- correlation coefficient R. b. Temporal evolution of the enha ues. The background valuesobtained (Fig. by 4 smoothing left the panel minimumserved in of in blue) the 10 total were day masses intervals. ob- The resulting burdens are plotte Fig. 3. both species as red and blue lines, respectively. The values Y. R’Honi et al.: Exceptional emissions of 220 225 230 235 240