Journal
GEOPHYSICAL RESEARCH LETTERS
Volume 42, Issue 8, Pages 3063-3068Publisher
AMER GEOPHYSICAL UNION
DOI: 10.1002/2015GL063142
Keywords
SOA; hygroscopicity; adsorption; solubility; aerosol
Categories
Funding
- Academy of Finland [272041, 259005, 267514, 139656]
- European Research Council [335478, 278277, 227463]
- European Union [BACCHUS: 603445, PEGASOS: 265148, ACTRIS: 262254]
- Nordforsk via Nordic Center of Excellence CRAICC
- University of Eastern Finland
- U.S. Office of Science (BER), Department of Energy [DE-SC0006980, DE-SC0011935, DE-FG02-05ER63995]
- U.S. National Science Foundation Atmospheric Chemistry Program [AGS-1244918, AGS-1244999]
- NASA [NNX-12AE54G]
- Academy of Finland (AKA) [267514, 267514] Funding Source: Academy of Finland (AKA)
- European Research Council (ERC) [335478] Funding Source: European Research Council (ERC)
- Directorate For Geosciences
- Div Atmospheric & Geospace Sciences [1244999] Funding Source: National Science Foundation
- U.S. Department of Energy (DOE) [DE-SC0011935, DE-SC0006980] Funding Source: U.S. Department of Energy (DOE)
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Aerosol climate effects are intimately tied to interactions with water. Here we combine hygroscopicity measurements with direct observations about the phase of secondary organic aerosol (SOA) particles to show that water uptake by slightly oxygenated SOA is an adsorption-dominated process under subsaturated conditions, where low solubility inhibits water uptake until the humidity is high enough for dissolution to occur. This reconciles reported discrepancies in previous hygroscopicity closure studies. We demonstrate that the difference in SOA hygroscopic behavior in subsaturated and supersaturated conditions can lead to an effect up to about 30% in the direct aerosol forcinghighlighting the need to implement correct descriptions of these processes in atmospheric models. Obtaining closure across the water saturation point is therefore a critical issue for accurate climate modeling.
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