Look Up: Probing the Vertical Profile of New Particle Formation and Growth in the Planetary Boundary Layer With Models and Observations

O’Donnell, Samuel E.; Akherati, Ali; He, Yicong; Hodshire, Anna L.; Shilling, John E.; Kuang, Chongai; Fast, Jerome D.; Mei, Fan; Schobesberger, Siegfried; Thornton, Joel A.; Smith, James N.; Jathar, Shantanu H.; Pierce, Jeffrey R.

doi:10.1029/2022JD037525

Title: Look Up: Probing the Vertical Profile of New Particle Formation and Growth in the Planetary Boundary Layer With Models and Observations

Journal Article · 27 January 2023 · Journal of Geophysical Research: Atmospheres

DOI: https://doi.org/10.1029/2022JD037525 · OSTI ID:1922528

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^[2]; He, Yicong ^[3];

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^[5]; Kuang, Chongai ^[6]; Fast, Jerome D. ^[5];

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^[8]; Smith, James N. ^[9];

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Department of Atmospheric Science Colorado State University Fort Collins CO USA
Ramboll USA, Inc. Arlington VA USA
State Key Joint Laboratory of Environment Simulation and Pollution Control Tsinghua University Beijing China
Handix Scientific Fort Collins CO USA
Pacific Northwest National Laboratory Richland WA USA
Brookhaven National Laboratory Upton NY USA
Department of Atmospheric Science University of Washington Seattle WA USA, Department of Applied Physics University of Eastern Finland Kuopio Finland
Department of Atmospheric Science University of Washington Seattle WA USA
Department of Chemistry University of California Irvine Irvine CA USA
Department of Mechanical Engineering Colorado State University Fort Collins CO USA

Abstract The processes of new particle formation (NPF) and growth are important contributors to cloud condensation nuclei (CCN) concentrations, and CCN are important for climate from their impact on planetary radiative forcing. While the general ubiquity and importance of NPF is understood, the vertical extent and governing mechanisms of NPF and growth in the lower troposphere are uncertain. We present an analysis of four NPF events and two non‐NPF events during the HI‐SCALE field campaign at the Southern Great Plains observatory in Oklahoma, USA. First, we analyzed airborne and ground‐based observations of aerosol and gas‐phase properties. Second, we used a column aerosol chemistry and microphysics model to probe factors that influence the vertical profile of NPF. During HI‐SCALE, we found several instances of enhanced NPF occurring several hundred meters above the surface; however, the spatio‐temporal characteristics of the observed NPF made comparisons between airborne‐ and ground‐based observations difficult. The model represented the observed NPF (or lack of NPF) and particle growth at the surface to final diameters within 10 nm. The model predicted enhanced NPF rates in the upper mixed layer, and this enhancement is primarily due to the temperature dependence in the NPF schemes, but this was also dependent on the vertical profile of gas‐phase precursors measured during HI‐SCALE. We found vertical mixing in the model either enhanced or suppressed NPF rates, aerosol number concentrations, and particle growth rates at the surface. Finally, our analysis provides insights for future field campaigns and modeling efforts investigating the vertical profile of NPF.

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Research Organization:: ARM Data Center, Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Oceanic and Atmospheric Administration (NOAA); USDOE; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC06-76RL01830; SC0012704; SC0017975; SC0019000; SC0021208

OSTI ID:: 1922528

Report Number(s):: BNL-223948-2023-JAAM; PNNL-SA-176018; e2022JD037525

Journal Information:: Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Journal Issue: 3 Vol. 128; ISSN 2169-897X

Publisher:: American Geophysical Union (AGU)Copyright Statement

Country of Publication:: United States

Language:: English

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Experimental investigation into the volatilities of highly oxygenated organic molecules (HOMs) Peräkylä, Otso; Riva, Matthieu; Heikkinen, Liine Atmospheric Chemistry and Physics, Vol. 20, Issue 2 https://doi.org/10.5194/acp-20-649-2020	journal	January 2020
Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air Tong, Haijie; Liu, Fobang; Filippi, Alexander Atmospheric Chemistry and Physics, Vol. 21, Issue 13 https://doi.org/10.5194/acp-21-10439-2021	journal	July 2021
Zeppelin-led study on the onset of new particle formation in the planetary boundary layer Lampilahti, Janne; Manninen, Hanna E.; Nieminen, Tuomo Atmospheric Chemistry and Physics, Vol. 21, Issue 16 https://doi.org/10.5194/acp-21-12649-2021	journal	August 2021
Aerosol characteristics at the Southern Great Plains site during the HI-SCALE campaign Liu, Jiumeng; Alexander, Liz; Fast, Jerome D. Atmospheric Chemistry and Physics, Vol. 21, Issue 6 https://doi.org/10.5194/acp-21-5101-2021	journal	January 2021
Aerosol particle formation in the upper residual layer Lampilahti, Janne; Leino, Katri; Manninen, Antti Atmospheric Chemistry and Physics, Vol. 21, Issue 10 https://doi.org/10.5194/acp-21-7901-2021	journal	May 2021
Determination of free amino acids, saccharides, and selected microbes in biogenic atmospheric aerosols – seasonal variations, particle size distribution, chemical and microbial relations Ruiz-Jimenez, Jose; Okuljar, Magdalena; Sietiö, Outi-Maaria Atmospheric Chemistry and Physics, Vol. 21, Issue 11 https://doi.org/10.5194/acp-21-8775-2021	journal	June 2021
Columnar modelling of nucleation burst evolution in the convective boundary layer – first results from a feasibility study Part I: Modelling approach Hellmuth, O. Atmospheric Chemistry and Physics, Vol. 6, Issue 12 https://doi.org/10.5194/acp-6-4175-2006	journal	September 2006
MALTE – model to predict new aerosol formation in the lower troposphere Boy, M.; Hellmuth, O.; Korhonen, H. Atmospheric Chemistry and Physics, Vol. 6, Issue 12 https://doi.org/10.5194/acp-6-4499-2006	journal	January 2006
Efficiency of cloud condensation nuclei formation from ultrafine particles Pierce, J. R.; Adams, P. J. Atmospheric Chemistry and Physics, Vol. 7, Issue 5 https://doi.org/10.5194/acp-7-1367-2007	journal	January 2007
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity Petters, M. D.; Kreidenweis, S. M. Atmospheric Chemistry and Physics, Vol. 7, Issue 8 https://doi.org/10.5194/acp-7-1961-2007	journal	January 2007
Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates Pierce, J. R.; Adams, P. J. Atmospheric Chemistry and Physics, Vol. 9, Issue 4 https://doi.org/10.5194/acp-9-1339-2009	journal	January 2009
HOVERCAT: a novel aerial system for evaluation of aerosol–cloud interactions Creamean, Jessie M.; Primm, Katherine M.; Tolbert, Margaret A. Atmospheric Measurement Techniques, Vol. 11, Issue 7 https://doi.org/10.5194/amt-11-3969-2018	journal	January 2018
Evaluating the performance of five different chemical ionization techniques for detecting gaseous oxygenated organic species Riva, Matthieu; Rantala, Pekka; Krechmer, Jordan E. Atmospheric Measurement Techniques, Vol. 12, Issue 4 https://doi.org/10.5194/amt-12-2403-2019	journal	January 2019
Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model Jathar, S. H.; Cappa, C. D.; Wexler, A. S. Geoscientific Model Development, Vol. 8, Issue 8 https://doi.org/10.5194/gmd-8-2553-2015	journal	January 2015

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