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Title: Examining the vertical heterogeneity of aerosols over the Southern Great Plains

Journal Article · · Atmospheric Chemistry and Physics (Online)

Atmospheric aerosols affect the global energy budget by scattering and absorbing sunlight (direct effects) and by changing the microphysical structure, lifetime, and coverage of clouds (indirect effects). Both aerosol direct and indirect effects are affected by the vertical distribution of aerosols in the atmosphere, which is further influenced by a range of processes, such as aerosol dynamics, long-range transport, and entrainment. However, many observations of these processes are based on ground measurements, limiting our ability to understand the vertical distribution of aerosols and simulate their impact on clouds and climate. In this work, we examined the vertical heterogeneity of aerosols over the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) using data collected from the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign. The vertical profiles of meteorological and aerosol physiochemical properties up to 2500 m above are examined based on the 38 flights conducted during the HI-SCALE campaign. The aerosol properties over the SGP show strong vertical heterogeneity and seasonal variabilities. The aerosol concentrations at the surface are the highest due to strong emissions at ground level. In general, the mode diameter of aerosols during summer (~ 100 nm) is larger than that during spring (~ 30 nm), a result of enhanced condensational growth due to enriched volatile organic compounds in summer. The concentration of aerosols below 30 nm in the boundary layer (BL) (e.g., below 1000 m) during spring is higher than that during summer, a result of the stronger new particle formation (NPF) events due to the reduced condensation sink in spring. In the BL, the size of the aerosols gradually increases with altitude due to condensational growth and cloud processing. However, the chemical composition of the aerosols remained similar, with organics and sulfates representing 59.8 ± 2.2 % and 22.7 ± 2.1 %, respectively, of the total mass in the BL. Through the vertical profiles of aerosol properties, we observed NPF events in the upper BL during 7 out of 38 research flights, where the newly formed particles continue to grow as they are mixed down to the surface. There is also an indication that deep convection brings aerosols from the free troposphere (FT) to the surface, where they grow to contribute to the cloud condensation nuclei (CCN). Overall, the vertical heterogeneity of aerosols over the SGP is influenced by aerosol dynamics (new particle formation, growth, and cloud processing) and transport processes (mixing in the BL, long-range transport, entrainment, and convective downward transport). Case studies showing the influence of these factors are discussed.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Brookhaven National Laboratory (BNL), Upton, NY (United States); Environmental Molecular Sciences Laboratory (EMSL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Contributing Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Grant/Contract Number:
SC0021256; 49297; 48804; AC05-76RL01830; SC0048804; SC0049297; SC0012704
OSTI ID:
2246957
Alternate ID(s):
OSTI ID: 2263348; OSTI ID: 2283970; OSTI ID: 2319177
Report Number(s):
PNNL-SA-184366; BNL-225364-2024-JAAM
Journal Information:
Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 23 Journal Issue: 24; ISSN 1680-7324
Publisher:
Copernicus GmbHCopyright Statement
Country of Publication:
Germany
Language:
English

References (38)

Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM) journal April 2015
Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer journal January 2007
The Atmospheric Radiation Measurement Program journal January 2003
The DOE ARM Aerial Facility journal May 2014
Unexpectedly high aerosol load in the free troposphere over central Europe in spring/summer 2003 journal November 2003
Cloud condensation nuclei characteristics at the Southern Great Plains site: role of particle size distribution and aerosol hygroscopicity journal July 2021
Determination of cloud condensation nuclei production from measured new particle formation events journal January 2009
Vertically resolved concentration and liquid water content of atmospheric nanoparticles at the US DOE Southern Great Plains site journal January 2018
Aerosol characteristics at the Southern Great Plains site during the HI-SCALE campaign journal January 2021
Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site journal January 2016
Cold Air Outbreaks Promote New Particle Formation Off the U.S. East Coast journal March 2022
New particle formation in the free troposphere: A question of chemistry and timing journal May 2016
Reevaluating the contribution of sulfuric acid and the origin of organic compounds in atmospheric nanoparticle growth journal December 2015
Dependence of nucleation rates on sulfuric acid vapor concentration in diverse atmospheric locations journal January 2008
Quantifying aerosol size distributions and their temporal variability in the Southern Great Plains, USA journal January 2019
New particle formation in the remote marine boundary layer journal January 2021
A new balance formula to estimate new particle formation rate: reevaluating the effect of coagulation scavenging journal January 2017
Using aircraft measurements to characterize subgrid-scale variability of aerosol properties near the Atmospheric Radiation Measurement Southern Great Plains site journal September 2022
Rapid measurement of sub-micrometer aerosol size distribution using a fast integrated mobility spectrometer journal July 2018
Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition journal January 2021
Temporal variation of aerosol properties at a rural continental site and study of aerosol evolution through growth law analysis journal January 2006
The Characteristics of Tropical and Midlatitude Mesoscale Convective Systems as Revealed by Radar Wind Profilers journal April 2019
The Arm Climate Research Facility: A Review of Structure and Capabilities journal March 2013
The use of trajectory cluster analysis to examine the long-range transport of secondary inorganic aerosol in the UK journal November 2005
Isoprene suppression of new particle formation: Potential mechanisms and implications: ISOPRENE SUPPRESSION OF NPF journal December 2016
Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States journal December 2014
Cloud Condensation Nuclei Closure Study Using Airborne Measurements Over the Southern Great Plains journal February 2023
Look Up: Probing the Vertical Profile of New Particle Formation and Growth in the Planetary Boundary Layer With Models and Observations journal January 2023
Exploring Stratocumulus Cloud-Top Entrainment Processes and Parameterizations by Using Doppler Cloud Radar Observations journal February 2016
Seasonal differences in the vertical profiles of aerosol optical properties over rural Oklahoma journal January 2011
Aerosol particle formation in the upper residual layer journal May 2021
A large source of cloud condensation nuclei from new particle formation in the tropics journal October 2019
Observation of ambient aerosol particle growth due to in-cloud processes within boundary layers journal January 2007
Diurnal evolution of negative atmospheric ions above the boreal forest: from ground level to the free troposphere journal July 2022
Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall journal October 2016
Molecular understanding of the suppression of new-particle formation by isoprene journal January 2020
New fast integrated mobility spectrometer for real-time measurement of aerosol size distribution—I: Concept and theory journal October 2006
ARM Southern Great Plains Site Observations of the Smoke Pall Associated with the 1998 Central American Fires journal November 2000

Figures / Tables (15)