Optical properties and composition of viscous organic particles found in the Southern Great Plains

<p>Atmospheric high-viscosity organic particles (HVOPs) were observed in samples of ambient aerosols collected in April and May 2016 in the Southern Great Plains of the United States. These particles were apportioned as either airborne soil organic particles (ASOPs) or tar balls (TBs) from bio...

Full description

Bibliographic Details
Main Authors: M. Fraund, D. J. Bonanno, S. China, D. Q. Pham, D. Veghte, J. Weis, G. Kulkarni, K. Teske, M. K. Gilles, A. Laskin, R. C. Moffet
Format: Article
Language:English
Published: Copernicus Publications 2020-10-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/20/11593/2020/acp-20-11593-2020.pdf
id doaj-303605a3903e40b3880bb66bc6b0921d
record_format Article
collection DOAJ
language English
format Article
sources DOAJ
author M. Fraund
D. J. Bonanno
S. China
D. Q. Pham
D. Veghte
J. Weis
J. Weis
J. Weis
G. Kulkarni
K. Teske
M. K. Gilles
A. Laskin
A. Laskin
R. C. Moffet
R. C. Moffet
spellingShingle M. Fraund
D. J. Bonanno
S. China
D. Q. Pham
D. Veghte
J. Weis
J. Weis
J. Weis
G. Kulkarni
K. Teske
M. K. Gilles
A. Laskin
A. Laskin
R. C. Moffet
R. C. Moffet
Optical properties and composition of viscous organic particles found in the Southern Great Plains
Atmospheric Chemistry and Physics
author_facet M. Fraund
D. J. Bonanno
S. China
D. Q. Pham
D. Veghte
J. Weis
J. Weis
J. Weis
G. Kulkarni
K. Teske
M. K. Gilles
A. Laskin
A. Laskin
R. C. Moffet
R. C. Moffet
author_sort M. Fraund
title Optical properties and composition of viscous organic particles found in the Southern Great Plains
title_short Optical properties and composition of viscous organic particles found in the Southern Great Plains
title_full Optical properties and composition of viscous organic particles found in the Southern Great Plains
title_fullStr Optical properties and composition of viscous organic particles found in the Southern Great Plains
title_full_unstemmed Optical properties and composition of viscous organic particles found in the Southern Great Plains
title_sort optical properties and composition of viscous organic particles found in the southern great plains
publisher Copernicus Publications
series Atmospheric Chemistry and Physics
issn 1680-7316
1680-7324
publishDate 2020-10-01
description <p>Atmospheric high-viscosity organic particles (HVOPs) were observed in samples of ambient aerosols collected in April and May 2016 in the Southern Great Plains of the United States. These particles were apportioned as either airborne soil organic particles (ASOPs) or tar balls (TBs) from biomass burning based on spetro-microscopic imaging and assessments of meteorological records of smoke and precipitation data. Regardless of their apportionment, the number fractions of HVOPs were positively correlated (<span class="inline-formula"><i>R</i><sup>2</sup>=0.85</span>) with increased values of absorption Ångström exponent (AAE) measured in situ for ambient aerosol at the site. Extending this correlation to 100&thinsp;% HVOPs yields an AAE of 2.6, similar to previous literature reports of the class of light-absorbing organic particles known as brown carbon (<span class="inline-formula">BrC</span>). One out of the three samples investigated had a significant number of ASOPs, while the other two samples contained TBs. Although there are chemical similarities between ASOPs and TBs, they can be distinguished based on composition inferred from near-edge absorption X-ray fine structure (NEXAFS) spectroscopy. ASOPs were distinguished from TBs based on their average <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M3" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><mo>-</mo><mi mathvariant="normal">COOH</mi><mo>/</mo><mi mathvariant="normal">C</mi><mo>=</mo><mi mathvariant="normal">C</mi></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="72pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="a49069135227ba155a11fcf3cc8deeea"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-20-11593-2020-ie00001.svg" width="72pt" height="14pt" src="acp-20-11593-2020-ie00001.png"/></svg:svg></span></span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M4" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><mo>-</mo><mi mathvariant="normal">COOH</mi><mo>/</mo><mi mathvariant="normal">COH</mi></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="73pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="f25071a5ae15323f7a74a7767f7f3ece"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-20-11593-2020-ie00002.svg" width="73pt" height="14pt" src="acp-20-11593-2020-ie00002.png"/></svg:svg></span></span> peak ratios, with ASOPs having lower ratios. NEXAFS spectra of filtered soil organic brine particles nebulized from field samples of standing water deposited after rain were consistent with ASOPs when laboratory particles were generated by bubble bursting at the air–organic brine interface. However, particles generated by nebulizing the bulk volume of soil organic brine had a particle composition different from ASOPs. These observations are consistent with the raindrop generation mechanism responsible for ASOP emissions in the area of study. In contrast, nebulized samples carry with them higher fractions of soil inorganics dissolved in the bulk volume of soil brine, which are not aerosolized by the raindrop mechanism. Our results support the bubble bursting mechanism of particle generation during rainfall resulting in the ejection of soil organics into the atmosphere. In addition, our results show that ASOPs may only be atmospherically relevant during times when suitable emission conditions are met.</p>
url https://acp.copernicus.org/articles/20/11593/2020/acp-20-11593-2020.pdf
work_keys_str_mv AT mfraund opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT djbonanno opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT schina opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT dqpham opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT dveghte opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT jweis opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT jweis opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT jweis opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT gkulkarni opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT kteske opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT mkgilles opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT alaskin opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT alaskin opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT rcmoffet opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
AT rcmoffet opticalpropertiesandcompositionofviscousorganicparticlesfoundinthesoutherngreatplains
_version_ 1724422357715517440
spelling doaj-303605a3903e40b3880bb66bc6b0921d2020-11-25T04:09:19ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242020-10-0120115931160610.5194/acp-20-11593-2020Optical properties and composition of viscous organic particles found in the Southern Great PlainsM. Fraund0D. J. Bonanno1S. China2D. Q. Pham3D. Veghte4J. Weis5J. Weis6J. Weis7G. Kulkarni8K. Teske9M. K. Gilles10A. Laskin11A. Laskin12R. C. Moffet13R. C. Moffet14Department of Chemistry, University of the Pacific, Stockton, California 95204, USADepartment of Chemistry, University of the Pacific, Stockton, California 95204, USAEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory (PNNL), Richland, Washington 99352, USADepartment of Chemistry, University of the Pacific, Stockton, California 95204, USACenter for Electron Microscopy and Analysis, The Ohio State University, Columbus, Ohio 43212, USAChemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USADepartment of Chemistry, University of California, Berkeley, California 94720, USAcurrent address: Physikalisches Institut, Universität Würzburg, Am Hubland, 97074 Würzburg, GermanyEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory (PNNL), Richland, Washington 99352, USAAtmospheric Radiation Monitoring (Southern Great Plains Climate Research Facility), Billings, Oklahoma 74630, USAChemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USAEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory (PNNL), Richland, Washington 99352, USAcurrent address: Chemistry Department, Purdue University, West Lafayette, Indiana 47907, USADepartment of Chemistry, University of the Pacific, Stockton, California 95204, USAcurrent address: Sonoma Technology, Petaluma, California 94954, USA<p>Atmospheric high-viscosity organic particles (HVOPs) were observed in samples of ambient aerosols collected in April and May 2016 in the Southern Great Plains of the United States. These particles were apportioned as either airborne soil organic particles (ASOPs) or tar balls (TBs) from biomass burning based on spetro-microscopic imaging and assessments of meteorological records of smoke and precipitation data. Regardless of their apportionment, the number fractions of HVOPs were positively correlated (<span class="inline-formula"><i>R</i><sup>2</sup>=0.85</span>) with increased values of absorption Ångström exponent (AAE) measured in situ for ambient aerosol at the site. Extending this correlation to 100&thinsp;% HVOPs yields an AAE of 2.6, similar to previous literature reports of the class of light-absorbing organic particles known as brown carbon (<span class="inline-formula">BrC</span>). One out of the three samples investigated had a significant number of ASOPs, while the other two samples contained TBs. Although there are chemical similarities between ASOPs and TBs, they can be distinguished based on composition inferred from near-edge absorption X-ray fine structure (NEXAFS) spectroscopy. ASOPs were distinguished from TBs based on their average <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M3" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><mo>-</mo><mi mathvariant="normal">COOH</mi><mo>/</mo><mi mathvariant="normal">C</mi><mo>=</mo><mi mathvariant="normal">C</mi></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="72pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="a49069135227ba155a11fcf3cc8deeea"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-20-11593-2020-ie00001.svg" width="72pt" height="14pt" src="acp-20-11593-2020-ie00001.png"/></svg:svg></span></span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M4" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><mo>-</mo><mi mathvariant="normal">COOH</mi><mo>/</mo><mi mathvariant="normal">COH</mi></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="73pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="f25071a5ae15323f7a74a7767f7f3ece"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-20-11593-2020-ie00002.svg" width="73pt" height="14pt" src="acp-20-11593-2020-ie00002.png"/></svg:svg></span></span> peak ratios, with ASOPs having lower ratios. NEXAFS spectra of filtered soil organic brine particles nebulized from field samples of standing water deposited after rain were consistent with ASOPs when laboratory particles were generated by bubble bursting at the air–organic brine interface. However, particles generated by nebulizing the bulk volume of soil organic brine had a particle composition different from ASOPs. These observations are consistent with the raindrop generation mechanism responsible for ASOP emissions in the area of study. In contrast, nebulized samples carry with them higher fractions of soil inorganics dissolved in the bulk volume of soil brine, which are not aerosolized by the raindrop mechanism. Our results support the bubble bursting mechanism of particle generation during rainfall resulting in the ejection of soil organics into the atmosphere. In addition, our results show that ASOPs may only be atmospherically relevant during times when suitable emission conditions are met.</p>https://acp.copernicus.org/articles/20/11593/2020/acp-20-11593-2020.pdf