Anthropogenic extremely low volatility organics (ELVOCs) Govern the Growth of Molecular Clusters over the Southern Great Plains during the Springtime

Shrivastava, ManishKumar B.; Zhang, Jie; Zaveri, Rahul A.; Zhao, Bin; Pierce, Jeffrey; O'Donnell, Samuel; Fast, Jerome D.; Gaudet, Brian J.; Shilling, John E.; Zelenyuk-Imre, Alla; Murphy, Benjamin N.; Pye, Havala O.; Zhang, Qi; Trousdell, Justin; Zhang, Renyi; Li, Yixin; Chen, Qi

doi:10.1029/2024JD041212

Anthropogenic extremely low volatility organics (ELVOCs) Govern the Growth of Molecular Clusters over the Southern Great Plains during the Springtime

Journal Article · 15 November 2024 · Journal of Geophysical Research: Atmospheres

DOI:https://doi.org/10.1029/2024JD041212· OSTI ID:2475274

^[1]; Zhang, Jie ^[1]; ^[1]; Zhao, Bin ^[2]; Pierce, Jeffrey ^[3]; O'Donnell, Samuel ^[3]; Fast, Jerome D. ^[1]; ^[1]; ^[1]; ^[1]; Murphy, Benjamin N. ^[4]; Pye, Havala O. ^[5]; Zhang, Qi ^[6]; Trousdell, Justin ^[7]; Zhang, Renyi ^[8]; Li, Yixin ^[8]; Chen, Qi ^[9]

BATTELLE (PACIFIC NW LAB)
Tsinghua University
Colorado State University
U.S. Environmental Protection Agency
US Environmental Protection Agency
University of California
University of California, Davis
Texas A & M University
Peking University

New particle formation (NPF) and growth govern cloud condensation nuclei (CCN) concentrations in many regions. The mechanisms governing the nucleation of molecular clusters vary substantially in different regions of the atmosphere. Additionally, the growth of these clusters from ~2 to 20 nm sizes is often governed by the availability of extremely low volatility organic vapours (ELVOCs). While the pathways to ELVOC formation from the oxidation of biogenic monoterpenes with ozone is better understood, the chemical and mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are not well understood. We integrate measurements and three-dimensional regional model simulations with the Weather Research and Forecasting Model coupled to chemistry (WRF-Chem) to understand the processes governing new particle formation and growth and secondary organic aerosol (SOA) formation during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) field campaign at the Southern Great Plains (SGP) observatory in Oklahoma, and contrast it with a site within the Bankhead National Forest (BNF), Alabama in Southeast USA, where 5-year long measurements will begin in 2024. Simulations show that nucleation rates are at least an order of magnitude higher at SGP compared to BNF during the springtime days (April 28 and May 14, 2016), largely due to lower H2SO4 concentrations at BNF, which are needed for nucleation. In addition, the larger CS at BNF (compared to SGP) increase the loss of molecular clusters by coagulation to pre-existing particles. Among the 8 different nucleation mechanisms in WRF-Chem, we find that the amine+H2SO4 nucleation mechanism dominates at the SGP site, while the pure organic ion induced nucleation mechanism dominates over BNF. Through various WRF-Chem sensitivity simulations, we find that anthropogenic ELVOCs are critical for explaining the growth of newly formed particles and the resulting number size distribution observed near the surface at the SGP site during the daytime. In addition, we show that treating organic particles as semisolid, with strong diffusion-limited uptake of organic vapours, brings model predictions into closer agreement with the observed evolution of particle size distribution. Simulations also predict that anthropogenic SOA, formed by the oxidation of aromatic volatile organic compounds (VOCs), is the dominant organic aerosol component at SGP, while biogenic SOA dominates particle composition at the BNF site in Southeast USA on these days.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 2475274

Report Number(s):: PNNL-SA-195923

Journal Information:: Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Journal Issue: 21 Vol. 129

Country of Publication:: United States

Language:: English

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