期刊
ATMOSPHERIC CHEMISTRY AND PHYSICS
卷 18, 期 2, 页码 845-863出版社
COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-18-845-2018
关键词
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资金
- German Federal Ministry of Education and Research [01LK1222A]
- Marie Curie Initial Training Network CLOUD-TRAIN [316662]
- US Department of Energy's Atmospheric System Research program
- Office of Science, Office of Biological and Environmental Research [DE-SC0011780]
- Swiss National Science Foundation [P2EZP2_168787]
- NSF [1439551, 1602086]
- Academy of Finland [299574]
- European Union's Horizon research and innovation program under the Marie Sklodowska-Curie grant [656994]
- U.S. Department of Energy (DOE) [DE-SC0011780] Funding Source: U.S. Department of Energy (DOE)
- Directorate For Geosciences
- Div Atmospheric & Geospace Sciences [1439551, 1602086] Funding Source: National Science Foundation
- Swiss National Science Foundation (SNF) [P2EZP2_168787] Funding Source: Swiss National Science Foundation (SNF)
A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (similar to 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38% relative humidity, sulfuric acid concentration between 1 x 10(6) and 3 x 10(7) cm(-3), and dimethylamine mixing ratio of similar to 40 pptv, i.e., 1 x 10(9) cm(-3)).
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