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DOI | 10.5194/acp-18-17451-2018 |
H2SO4-H2O-NH3 ternary ion-mediated nucleation (TIMN): kinetic-based model and comparison with CLOUD measurements | |
Yu, Fangqun1; Nadykto, Alexey B.1,2,3; Herb, Jason1; Luo, Gan1; Nazarenko, Kirill M.2; Uvarova, Lyudmila A.2,3 | |
2018-12-10 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:23页码:17451-17474 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Russia |
英文摘要 | New particle formation (NPF) is known to be an important source of atmospheric particles that impacts air quality, hydrological cycle, and climate. Although laboratory measurements indicate that ammonia enhances NPF, the physicochemical processes underlying the observed effect of ammonia on NPF are yet to be understood. Here we present a comprehensive kinetically based H2SO4-H2O-NH3 ternary ion-mediated nucleation (TIMN) model that is based on the thermodynamic data derived from both quantum-chemical calculations and laboratory measurements. NH3 was found to reduce nucleation barriers for neutral, positively charged, and negatively charged clusters differently, due to large differences in the binding strength of NH3, H2O, and H2SO4 to small clusters of different charging states. The model reveals the general favor of nucleation of negative ions, followed by nucleation on positive ions and neutral nucleation, for which higher NH3 concentrations are needed, in excellent agreement with Cosmics Leaving OUtdoor Droplets (CLOUD) measurements. The TIMN model explicitly resolves dependences of nucleation rates on all the key controlling parameters and captures the absolute values of nucleation rates as well as the dependence of TIMN rates on concentrations of NH3 and H2SO4, ionization rates, temperature, and relative humidity observed in the well-controlled CLOUD measurements well. The kinetic model offers physicochemical insights into the ternary nucleation process and provides a physics-based approach to calculate TIMN rates under a wide range of atmospheric conditions. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000452661400003 |
WOS关键词 | INDUCED AEROSOL FORMATION ; SULFURIC-ACID DIMERS ; GAS-PHASE ; MOLECULAR CLUSTERS ; PARTICLE NUCLEATION ; EXPERIMENTAL THERMODYNAMICS ; BINDING-ENERGIES ; OXALIC-ACID ; AMMONIA ; HYDRATION |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/30749 |
专题 | 地球科学 |
作者单位 | 1.SUNY Albany, Atmospher Sci Res Ctr, Albany, NY 12222 USA; 2.Moscow State Univ Technol STANKIN, Dept Appl Math, Moscow, Russia; 3.Natl Res Nucl Univ, MEPhI Moscow Engn Phys Inst, Dept Gen Phys, Moscow, Russia |
推荐引用方式 GB/T 7714 | Yu, Fangqun,Nadykto, Alexey B.,Herb, Jason,et al. H2SO4-H2O-NH3 ternary ion-mediated nucleation (TIMN): kinetic-based model and comparison with CLOUD measurements[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(23):17451-17474. |
APA | Yu, Fangqun,Nadykto, Alexey B.,Herb, Jason,Luo, Gan,Nazarenko, Kirill M.,&Uvarova, Lyudmila A..(2018).H2SO4-H2O-NH3 ternary ion-mediated nucleation (TIMN): kinetic-based model and comparison with CLOUD measurements.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(23),17451-17474. |
MLA | Yu, Fangqun,et al."H2SO4-H2O-NH3 ternary ion-mediated nucleation (TIMN): kinetic-based model and comparison with CLOUD measurements".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.23(2018):17451-17474. |
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