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Articles and Also and Instrumental Development Atmos. Chem. Phys., 19, 12631–12686, 2019 https://doi.org/10.5194/acp-19-12631-2019 © Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License. A review of experimental techniques for aerosol hygroscopicity studies Mingjin Tang1, Chak K. Chan2, Yong Jie Li3, Hang Su4,5, Qingxin Ma6, Zhijun Wu7, Guohua Zhang1, Zhe Wang8, Maofa Ge9, Min Hu7, Hong He6,10,11, and Xinming Wang1,10,11 1State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China 2School of Energy and Environment, City University of Hong Kong, Kowloon, Hong Kong, China 3Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Avenida da Universidade, Taipa, Macau, China 4Center for Air Pollution and Climate Change Research, Institute for Environmental and Climate Research, Jinan University, Guangzhou 511443, China 5Department of Multiphase Chemistry, Max Planck Institute for Chemistry, Mainz 55118, Germany 6State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China 7State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China 8Department of Civil and Environmental Engineering, Hong Kong Polytechnic University, Hong Kong, China 9State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China 10University of Chinese Academy of Sciences, Beijing 100049, China 11Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China Correspondence: Mingjin Tang ([email protected]) and Chak K. Chan ([email protected]) Received: 26 April 2019 – Discussion started: 3 May 2019 Revised: 26 August 2019 – Accepted: 16 September 2019 – Published: 10 October 2019 Abstract. Hygroscopicity is one of the most important are outlined and discussed for further technical improvement physicochemical properties of aerosol particles and also and instrumental development. plays indispensable roles in many other scientific and techni- cal fields. A myriad of experimental techniques, which differ in principles, configurations and cost, are available for in- vestigating aerosol hygroscopicity under subsaturated condi- 1 Introduction tions (i.e., relative humidity below 100 %). A comprehensive review of these techniques is provided in this paper, in which Aerosol particles are airborne solid or liquid particles in the experimental techniques are broadly classified into four cate- size range of a few nanometers to tens of micrometers. They gories, according to the way samples under investigation are can be emitted directly into the atmosphere (primary parti- prepared. For each technique, we describe its operation prin- cles) and can also be formed in the atmosphere (secondary ciple and typical configuration, use representative examples particles) by chemical transformation of gaseous precursors reported in previous work to illustrate how this technique can such as SO2, NOx, and volatile organic compounds (Pöschl, help better understand aerosol hygroscopicity, and discuss its 2005; Seinfeld and Pandis, 2016). Aerosol particles are of advantages and disadvantages. In addition, future directions great concern due to their environmental, health, climatic and biogeochemical impacts (Finlayson-Pitts and Pitts, 2000; Published by Copernicus Publications on behalf of the European Geosciences Union. 12632 M. Tang et al.: Aerosol hygroscopicity measurement techniques Jickells et al., 2005; Mahowald, 2011; Mahowald et al., 2011; cence of multicomponent particles can be more complicated IPCC, 2013; Pöschl and Shiraiwa, 2015; Seinfeld and Pandis, (Seinfeld and Pandis, 2016). 2016; Shiraiwa et al., 2017b). It should be pointed out that not all the single-component Water, which can exist in gas, liquid and solid states, is particles exhibit distinctive deliquescence and efflorescence. ubiquitous in the troposphere. Interactions of water vapor Instead, continuous uptake or loss of liquid water is ob- with aerosol particles largely affect the roles that aerosol par- served during humidification and dehumidification processes ticles play in the Earth system. When water vapor is supersat- for many inorganic and organic particles (Mikhailov et al., urated (i.e., when relative humidity, RH, is > 100 %), aerosol 2009; Koop et al., 2011; Shiraiwa et al., 2011). Particles particles can act as cloud condensation nuclei (CCN) to form with extremely low hygroscopicity (e.g., mineral dust) will cloud droplets and as ice-nucleating particles (INPs) to form not be deliquesced even at very high RH; instead, adsorbed ice crystals (Pruppacher and Klett, 1997; Lohmann and Fe- water will be formed on the particle surface (Tang et al., ichter, 2005; Vali et al., 2015; Lohmann et al., 2016; Tang 2016a). Furthermore, a multicomponent particle which con- et al., 2016a, 2018; Knopf et al., 2018). Cloud condensation tains some types of organic materials may undergo liquid– nucleation and ice nucleation activities of aerosol particles, liquid phase separation, leading to the formation of two co- as well as relevant experimental techniques, have been re- existing liquid phases in one particle (Mikhailov et al., 2009; cently reviewed in several books and review papers (Prup- You et al., 2012, 2014; Freedman, 2017; Song et al., 2017, pacher and Klett, 1997; Hoose and Moehler, 2012; Murray 2018). It is conventionally assumed that hygroscopic equilib- et al., 2012; Kreidenweis and Asa-Awuku, 2014; Farmer et rium of aerosol particles can be quickly reached. Neverthe- al., 2015; Lohmann et al., 2016; Tang et al., 2016a; Kanji et less, recent laboratory, field and modeling studies suggested al., 2017) and are thus not further discussed in this paper. that atmospherically relevant particles can be semi-solid or When water vapor is unsaturated (i.e., RH < 100 %), an amorphous solid (Virtanen et al., 2010; Zobrist et al., 2011; aerosol particle in equilibrium with the surrounding environ- Renbaum-Wolff et al., 2013; Shiraiwa et al., 2017a; Reid et ment would contain some amount of absorbed or adsorbed al., 2018). The viscosity of these particles can be high enough water (Martin, 2000; Kreidenweis and Asa-Awuku, 2014; such that uptake or release of water is largely limited by dif- Cheng et al., 2015; Farmer et al., 2015; Seinfeld and Pan- fusion of water molecules in the bulk phase of these particles. dis, 2016; Tang et al., 2016a; Freedman, 2017). The amount Hygroscopicity determines the amount of water that a par- of water that a particle contains depends on RH, tempera- ticle contains under a given condition and thereby has several ture, and its chemical composition and size. The ability of a important implications. It determines the size and refractive substance to absorb/adsorb water as a function of RH is typ- indices of aerosol particles, affecting their optical properties ically termed hygroscopicity (Adams and Merz, 1929; Su et and consequently their impacts on visibility and direct radia- al., 2010; Kreidenweis and Asa-Awuku, 2014; Tang et al., tive forcing (Malm and Day, 2001; Chin et al., 2002; Quinn et 2016a), and the underlying thermodynamic principles can be al., 2005; Hand and Malm, 2007; Cheng et al., 2008; Eichler found elsewhere (Martin, 2000; Seinfeld and Pandis, 2016). et al., 2008; Liu et al., 2012; Liu et al., 2013b; Brock et al., A single-component particle which contains a water-soluble 2016b; Titos et al., 2016; Haarig et al., 2017). Hygroscop- inorganic salt, such as .NH4/2SO4 and NaCl, is solid at low icity is also closely related to the CCN activity of aerosol RH. When RH is increased to the deliquescence relative hu- particles, affecting their impacts on formation and proper- midity (DRH), the solid particle will undergo deliquescence ties of clouds and thus their indirect radiative forcing (Mc- to form an aqueous particle, and the aqueous particle at DRH Figgans et al., 2006; Petters and Kreidenweis, 2007; Reut- is composed of a saturated solution (Cheng et al., 2015). ter et al., 2009; Kreidenweis and Asa-Awuku, 2014; Farmer Further increase in RH would increase the water content of et al., 2015). Aerosol liquid water and/or surface-adsorbed the aqueous droplet; i.e., the aqueous particle would become water, largely controlled by hygroscopicity, determine het- more diluted as RH increases. During humidification thermo- erogeneous and multiphase reactions of aerosol particles via dynamics determines the phase transition and hygroscopic several mechanisms, as revealed by recent studies (Bertram growth of the particle. During dehumidification, an aqueous and Thornton, 2009; Shiraiwa et al., 2011; Rubasinghege and particle would not undergo efflorescence to form a solid par- Grassian, 2013; Cheng et al., 2016; Wang et al., 2016; Tang ticle when RH is decreased to below DRH; instead, the aque- et al., 2017; Mu et al., 2018; Wu et al., 2018). In addition, ous particle would become supersaturated (i.e., the aqueous hygroscopicity significantly impacts dry and wet deposition particle becomes a supersaturated solution). Only when RH rates of aerosol particles and thus their lifetimes, spatiotem- is further
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