Manish Shrivastava, Jie Zhang, Rahul A. Zaveri, Bin Zhao, Jeffrey R. Pierce, Samuel E. O’Donnell, Jerome D. Fast, Brian Gaudet, John E. Shilling, Alla Zelenyuk, Benjamin N. Murphy, Havala O. T. Pye, Qi Zhang, Justin Trousdell, Renyi Zhang, Yixin Li, Qi Chen
{"title":"人类活动产生的极低挥发性有机物(ELVOC)控制着大平原南部春季分子集群的增长","authors":"Manish Shrivastava, Jie Zhang, Rahul A. Zaveri, Bin Zhao, Jeffrey R. Pierce, Samuel E. O’Donnell, Jerome D. Fast, Brian Gaudet, John E. Shilling, Alla Zelenyuk, Benjamin N. Murphy, Havala O. T. Pye, Qi Zhang, Justin Trousdell, Renyi Zhang, Yixin Li, Qi Chen","doi":"10.1029/2024JD041212","DOIUrl":null,"url":null,"abstract":"<p>New particle formation (NPF) often drives cloud condensation nuclei concentrations and the processes governing nucleation of molecular clusters vary substantially in different regions. The growth of these clusters from ∼2 to >10 nm diameters is often driven by the availability of extremely low volatility organic vapors (ELVOCs). Although the pathways to ELVOC formation from the oxidation of biogenic terpenes are better understood, the mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are less well understood. We integrate measurements and detailed regional model simulations to understand the processes governing NPF and secondary organic aerosol formation at the Southern Great Plain (SGP) observatory in Oklahoma and compare these with a site within the Bankhead National Forest (BNF) in Alabama, southeast USA. During our two simulated NPF event days, nucleation rates are predicted to be at least an order of magnitude higher at SGP compared to BNF largely due to lower sulfuric acid (H<sub>2</sub>SO<sub>4</sub>) concentrations at BNF. Among the different nucleation mechanisms in WRF-Chem, we find that the dimethylamine (DMA) + H<sub>2</sub>SO<sub>4</sub> nucleation mechanism dominates at SGP. We find that anthropogenic ELVOCs are critical for explaining the growth of particles observed at SGP. Treating organic particles as semisolid, with strong diffusion limitations for organic vapor uptake in the particle phase, brings model predictions into closer agreement with observations. We also simulate two non-NPF event days observed at the SGP site and show that low-level clouds reduce photochemical activity with corresponding reductions in H<sub>2</sub>SO<sub>4</sub> and anthropogenic ELVOC concentrations, thereby explaining the lack of NPF.</p>","PeriodicalId":15986,"journal":{"name":"Journal of Geophysical Research: Atmospheres","volume":"129 21","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1029/2024JD041212","citationCount":"0","resultStr":"{\"title\":\"Anthropogenic Extremely Low Volatility Organics (ELVOCs) Govern the Growth of Molecular Clusters Over the Southern Great Plains During the Springtime\",\"authors\":\"Manish Shrivastava, Jie Zhang, Rahul A. Zaveri, Bin Zhao, Jeffrey R. Pierce, Samuel E. O’Donnell, Jerome D. Fast, Brian Gaudet, John E. Shilling, Alla Zelenyuk, Benjamin N. Murphy, Havala O. T. Pye, Qi Zhang, Justin Trousdell, Renyi Zhang, Yixin Li, Qi Chen\",\"doi\":\"10.1029/2024JD041212\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>New particle formation (NPF) often drives cloud condensation nuclei concentrations and the processes governing nucleation of molecular clusters vary substantially in different regions. The growth of these clusters from ∼2 to >10 nm diameters is often driven by the availability of extremely low volatility organic vapors (ELVOCs). Although the pathways to ELVOC formation from the oxidation of biogenic terpenes are better understood, the mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are less well understood. We integrate measurements and detailed regional model simulations to understand the processes governing NPF and secondary organic aerosol formation at the Southern Great Plain (SGP) observatory in Oklahoma and compare these with a site within the Bankhead National Forest (BNF) in Alabama, southeast USA. During our two simulated NPF event days, nucleation rates are predicted to be at least an order of magnitude higher at SGP compared to BNF largely due to lower sulfuric acid (H<sub>2</sub>SO<sub>4</sub>) concentrations at BNF. Among the different nucleation mechanisms in WRF-Chem, we find that the dimethylamine (DMA) + H<sub>2</sub>SO<sub>4</sub> nucleation mechanism dominates at SGP. We find that anthropogenic ELVOCs are critical for explaining the growth of particles observed at SGP. Treating organic particles as semisolid, with strong diffusion limitations for organic vapor uptake in the particle phase, brings model predictions into closer agreement with observations. 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Anthropogenic Extremely Low Volatility Organics (ELVOCs) Govern the Growth of Molecular Clusters Over the Southern Great Plains During the Springtime
New particle formation (NPF) often drives cloud condensation nuclei concentrations and the processes governing nucleation of molecular clusters vary substantially in different regions. The growth of these clusters from ∼2 to >10 nm diameters is often driven by the availability of extremely low volatility organic vapors (ELVOCs). Although the pathways to ELVOC formation from the oxidation of biogenic terpenes are better understood, the mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are less well understood. We integrate measurements and detailed regional model simulations to understand the processes governing NPF and secondary organic aerosol formation at the Southern Great Plain (SGP) observatory in Oklahoma and compare these with a site within the Bankhead National Forest (BNF) in Alabama, southeast USA. During our two simulated NPF event days, nucleation rates are predicted to be at least an order of magnitude higher at SGP compared to BNF largely due to lower sulfuric acid (H2SO4) concentrations at BNF. Among the different nucleation mechanisms in WRF-Chem, we find that the dimethylamine (DMA) + H2SO4 nucleation mechanism dominates at SGP. We find that anthropogenic ELVOCs are critical for explaining the growth of particles observed at SGP. Treating organic particles as semisolid, with strong diffusion limitations for organic vapor uptake in the particle phase, brings model predictions into closer agreement with observations. We also simulate two non-NPF event days observed at the SGP site and show that low-level clouds reduce photochemical activity with corresponding reductions in H2SO4 and anthropogenic ELVOC concentrations, thereby explaining the lack of NPF.
期刊介绍:
JGR: Atmospheres publishes articles that advance and improve understanding of atmospheric properties and processes, including the interaction of the atmosphere with other components of the Earth system.