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...
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Copernicus Publications
2020-10-01
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Series: | Atmospheric Chemistry and Physics |
Online Access: | https://acp.copernicus.org/articles/20/11593/2020/acp-20-11593-2020.pdf |
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Article |
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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 % 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 |
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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 % 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 |