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| DOI | 10.5194/acp-19-5033-2019 |
| New particle formation from sulfuric acid and ammonia: Nucleation and growth model based on thermodynamics derived from CLOUD measurements for a wide range of conditions | |
| Kürten A. | |
| 发表日期 | 2019 |
| ISSN | 16807316 |
| 起始页码 | 5033 |
| 结束页码 | 5050 |
| 卷号 | 19期号:7 |
| 英文摘要 | Understanding new particle formation and growth is important because of the strong impact of these processes on climate and air quality. Measurements to elucidate the main new particle formation mechanisms are essential; however, these mechanisms have to be implemented in models to estimate their impact on the regional and global scale. Parameterizations are computationally cheap ways of implementing nucleation schemes in models, but they have their limitations, as they do not necessarily include all relevant parameters. Process models using sophisticated nucleation schemes can be useful for the generation of look-up tables in large-scale models or for the analysis of individual new particle formation events. In addition, some other important properties can be derived from a process model that implicitly calculates the evolution of the full aerosol size distribution, e.g., the particle growth rates. Within this study, a model (SANTIAGO - Sulfuric acid Ammonia NucleaTIon And GrOwth model) is constructed that simulates new particle formation starting from the monomer of sulfuric acid up to a particle size of several hundred nanometers. The smallest sulfuric acid clusters containing one to four acid molecules and a varying amount of base (ammonia) are allowed to evaporate in the model, whereas growth beyond the pentamer (five sulfuric acid molecules) is assumed to be entirely collision-controlled. The main goal of the present study is to derive appropriate thermodynamic data needed to calculate the cluster evaporation rates as a function of temperature. These data are derived numerically from CLOUD (Cosmics Leaving OUtdoor Droplets) chamber new particle formation rates for neutral sulfuric acid-water-ammonia nucleation at temperatures between 208 and 292K. The numeric methods include an optimization scheme to derive the best estimates for the thermodynamic data (dH and dS) and a Monte Carlo method to derive their probability density functions. The derived data are compared to literature values. Using different data sets for dH and dS in SANTIAGO detailed comparison between model results and measured CLOUD new particle formation rates is discussed. © 2019 Author(s). |
| 语种 | 英语 |
| scopus关键词 | aerosol; air quality; ammonia; atmospheric chemistry; climate effect; measurement method; nucleation; particle size; sulfuric acid; thermodynamics |
| 来源期刊 | Atmospheric Chemistry and Physics
 |
| 文献类型 | 期刊论文 |
| 条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/144488 |
| 作者单位 | Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, 60438, Germany |
| 推荐引用方式 GB/T 7714 | Kürten A.. New particle formation from sulfuric acid and ammonia: Nucleation and growth model based on thermodynamics derived from CLOUD measurements for a wide range of conditions[J],2019,19(7). |
| APA | Kürten A..(2019).New particle formation from sulfuric acid and ammonia: Nucleation and growth model based on thermodynamics derived from CLOUD measurements for a wide range of conditions.Atmospheric Chemistry and Physics,19(7). |
| MLA | Kürten A.."New particle formation from sulfuric acid and ammonia: Nucleation and growth model based on thermodynamics derived from CLOUD measurements for a wide range of conditions".Atmospheric Chemistry and Physics 19.7(2019). |
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