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Title: Enhanced light absorption by mixed source black and brown carbon particles in UK winter

Abstract

We report that black carbon (BC) and light-absorbing organic carbon (brown carbon, BrC) play key roles in warming the atmosphere, but the magnitude of their effects remains highly uncertain. Theoretical modelling and laboratory experiments demonstrate that coatings on BC can enhance BC’s light absorption, therefore many climate models simply assume enhanced BC absorption by a factor of ~1.5. However, recent field observations show negligible absorption enhancement, implying models may overestimate BC’s warming. Here we report direct evidence of substantial field-measured BC absorption enhancement, with the magnitude strongly depending on BC coating amount. Increases in BC coating result from a combination of changing sources and photochemical aging processes. When the influence of BrC is accounted for, observationally constrained model calculations of the BC absorption enhancement can be reconciled with the observations. In conclusion, we find that the influence of coatings on BC absorption should be treated as a source and regionally specific parameter in climate models.

Authors:
 [1];  [2];  [3];  [2];  [4];  [5];  [5];  [5];  [5];  [6];  [5];  [7];  [5];  [5];  [8];  [8]; ORCiD logo [8];  [9];  [9];  [10] more »;  [10];  [11];  [12]; ORCiD logo [13];  [14];  [15];  [16] « less
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Earth and Environmental Sciences Division; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences (CIRES)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Earth and Environmental Sciences Division
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Earth and Environmental Sciences Division; Carnegie Mellon Univ., Pittsburgh, PA (United States)
  4. Univ. of California, Davis, CA (United States)
  5. Aerodyne Research, Inc. Billerica, MA (United States)
  6. Aerodyne Research, Inc. Billerica, MA (United States); Univ. of Texas at Austin, Austin, TX (United States)
  7. Aerodyne Research, Inc. Billerica, MA (United States); Boston College, Boston, MA (United States)
  8. Michigan Technological Univ., Houghton, MI (United States)
  9. Georgia Inst. of Technology, Atlanta, GA (United States)
  10. Univ. of Manchester (United Kingdom)
  11. Univ. of York (United Kingdom)
  12. Univ. of Leicester (United Kingdom)
  13. Univ. of Washington, Seattle, WA (United States); Karlsruhe Inst. of Technology (KIT) (Germany)
  14. Paul Scherrer Inst. (PSI), Villigen (Switzerland); Lucerne University of Applied Sciences and Arts (Switzerland)
  15. Univ. of Bern, Bern (Switzerland)
  16. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Publication Date:
Research Org.:
Univ. of California, Davis, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1252985
Grant/Contract Number:  
SC0008937; SC0010019; SC0006002
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Liu, Shang, Aiken, Allison C., Gorkowski, Kyle, Dubey, Manvendra K., Cappa, Christopher D., Williams, Leah R., Herndon, Scott C., Massoli, Paola, Fortner, Edward C., Chhabra, Puneet S., Brooks, William A., Onasch, Timothy B., Jayne, John T., Worsnop, Douglas R., China, Swarup, Sharma, Noopur, Mazzoleni, Claudio, Xu, Lu, Ng, Nga L., Liu, Dantong, Allan, James D., Lee, James D., Fleming, Zoë L., Mohr, Claudia, Zotter, Peter, Szidat, Sönke, and Prévôt, André S. H. Enhanced light absorption by mixed source black and brown carbon particles in UK winter. United States: N. p., 2015. Web. doi:10.1038/ncomms9435.
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Liu, Shang, Aiken, Allison C., Gorkowski, Kyle, Dubey, Manvendra K., Cappa, Christopher D., Williams, Leah R., Herndon, Scott C., Massoli, Paola, Fortner, Edward C., Chhabra, Puneet S., Brooks, William A., Onasch, Timothy B., Jayne, John T., Worsnop, Douglas R., China, Swarup, Sharma, Noopur, Mazzoleni, Claudio, Xu, Lu, Ng, Nga L., Liu, Dantong, Allan, James D., Lee, James D., Fleming, Zoë L., Mohr, Claudia, Zotter, Peter, Szidat, Sönke, & Prévôt, André S. H. Enhanced light absorption by mixed source black and brown carbon particles in UK winter. United States. https://doi.org/10.1038/ncomms9435
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Liu, Shang, Aiken, Allison C., Gorkowski, Kyle, Dubey, Manvendra K., Cappa, Christopher D., Williams, Leah R., Herndon, Scott C., Massoli, Paola, Fortner, Edward C., Chhabra, Puneet S., Brooks, William A., Onasch, Timothy B., Jayne, John T., Worsnop, Douglas R., China, Swarup, Sharma, Noopur, Mazzoleni, Claudio, Xu, Lu, Ng, Nga L., Liu, Dantong, Allan, James D., Lee, James D., Fleming, Zoë L., Mohr, Claudia, Zotter, Peter, Szidat, Sönke, and Prévôt, André S. H. Wed . "Enhanced light absorption by mixed source black and brown carbon particles in UK winter". United States. https://doi.org/10.1038/ncomms9435. https://www.osti.gov/servlets/purl/1252985.
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@article{osti_1252985,
title = {Enhanced light absorption by mixed source black and brown carbon particles in UK winter},
author = {Liu, Shang and Aiken, Allison C. and Gorkowski, Kyle and Dubey, Manvendra K. and Cappa, Christopher D. and Williams, Leah R. and Herndon, Scott C. and Massoli, Paola and Fortner, Edward C. and Chhabra, Puneet S. and Brooks, William A. and Onasch, Timothy B. and Jayne, John T. and Worsnop, Douglas R. and China, Swarup and Sharma, Noopur and Mazzoleni, Claudio and Xu, Lu and Ng, Nga L. and Liu, Dantong and Allan, James D. and Lee, James D. and Fleming, Zoë L. and Mohr, Claudia and Zotter, Peter and Szidat, Sönke and Prévôt, André S. H.},
abstractNote = {We report that black carbon (BC) and light-absorbing organic carbon (brown carbon, BrC) play key roles in warming the atmosphere, but the magnitude of their effects remains highly uncertain. Theoretical modelling and laboratory experiments demonstrate that coatings on BC can enhance BC’s light absorption, therefore many climate models simply assume enhanced BC absorption by a factor of ~1.5. However, recent field observations show negligible absorption enhancement, implying models may overestimate BC’s warming. Here we report direct evidence of substantial field-measured BC absorption enhancement, with the magnitude strongly depending on BC coating amount. Increases in BC coating result from a combination of changing sources and photochemical aging processes. When the influence of BrC is accounted for, observationally constrained model calculations of the BC absorption enhancement can be reconciled with the observations. In conclusion, we find that the influence of coatings on BC absorption should be treated as a source and regionally specific parameter in climate models.},
doi = {10.1038/ncomms9435},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Wed Sep 30 00:00:00 EDT 2015},
month = {Wed Sep 30 00:00:00 EDT 2015}
}
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https://doi.org/10.1038/ncomms9435
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    Physicochemical Characteristics of Individual Aerosol Particles during the 2015 China Victory Day Parade in Beijing
    journal, January 2018

    Physical Properties of Aerosol Internally Mixed With Soot Particles in a Biogenically Dominated Environment in California
    journal, October 2018

    • Sharma, Noopur; China, Swarup; Bhandari, Janarjan
    • Geophysical Research Letters, Vol. 45, Issue 20
    • DOI: 10.1029/2018gl079404

    Morphological and radiative characteristics of soot aggregates: Experimental and numerical research
    journal, January 2020

    Production of particulate brown carbon during atmospheric aging of residential wood-burning emissions
    journal, January 2018

    • Kumar, Nivedita K.; Corbin, Joel C.; Bruns, Emily A.
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 24
    • DOI: 10.5194/acp-18-17843-2018

    Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition
    journal, February 2020

    • Fierce, Laura; Onasch, Timothy B.; Cappa, Christopher D.
    • Proceedings of the National Academy of Sciences, Vol. 117, Issue 10
    • DOI: 10.1073/pnas.1919723117

    Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments
    journal, March 2016

    • Peng, Jianfei; Hu, Min; Guo, Song
    • Proceedings of the National Academy of Sciences, Vol. 113, Issue 16
    • DOI: 10.1073/pnas.1602310113

    A novel approach to calibrating a photoacoustic absorption spectrometer using polydisperse absorbing aerosol
    journal, January 2019

    • Foster, Katie; Pokhrel, Rudra; Burkhart, Matthew
    • Atmospheric Measurement Techniques, Vol. 12, Issue 6
    • DOI: 10.5194/amt-12-3351-2019

    Investigation of the absorption Ångström exponent and its relation to physicochemical properties for mini-CAST soot
    text, January 2018

    Vertical characterization of aerosol optical properties and brown carbon in winter in urban Beijing, China
    journal, August 2018

    • Xie, Conghui; Xu, Weiqi; Wang, Junfeng
    • Atmospheric Chemistry and Physics Discussions
    • DOI: 10.5194/acp-2018-788

    Evidence of major secondary organic aerosol contribution to lensing effect black carbon absorption enhancement
    journal, December 2018

    • Zhang, Yunjiang; Favez, Olivier; Canonaco, Francesco
    • npj Climate and Atmospheric Science, Vol. 1, Issue 1
    • DOI: 10.1038/s41612-018-0056-2

    An inter-comparison of black-carbon-related instruments in a laboratory study of biomass burning aerosol
    text, January 2018

    On the accuracy of aerosol photoacoustic spectrometer calibrations using absorption by ozone
    journal, January 2018

    • Davies, Nicholas W.; Cottrell, Michael I.; Fox, Cathryn
    • Atmospheric Measurement Techniques Discussion
    • DOI: 10.5194/amt-2017-434

    Radiative effect and climate impacts of brown carbon with the Community Atmosphere Model (CAM5)
    journal, January 2018

    • Brown, Hunter; Liu, Xiaohong; Feng, Yan
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 24
    • DOI: 10.5194/acp-18-17745-2018

    Effects of brown coatings on the absorption enhancement of black carbon: a numerical investigation
    journal, January 2018

    Sources and physicochemical characteristics of black carbon aerosol from the southeastern Tibetan Plateau: internal mixing enhances light absorption
    journal, January 2018

    • Wang, Qiyuan; Cao, Junji; Han, Yongming
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 7
    • DOI: 10.5194/acp-18-4639-2018

    Optical properties of black carbon in cookstove emissions coated with secondary organic aerosols: Measurements and modeling
    journal, July 2016

    Extensive Soot Compaction by Cloud Processing from Laboratory and Field Observations
    journal, August 2019

    Quantification of online removal of refractory black carbon using laser-induced incandescence in the single particle soot photometer [Supplemental Data]
    preprint, April 2016

    • Aiken, Allison C.; McMeeking, Gavin R.; Levin, Ezra J. T.
    • figshare-Supplementary information for journal article at DOI: 10.1080/02786826.2016.1173647, 1 DOCX file (40.41 kB)
    • DOI: 10.6084/m9.figshare.3156049

    Aerosol absorption retrieval at ultraviolet wavelengths in a complex environment
    journal, January 2016

    • Kazadzis, Stelios; Raptis, Panagiotis; Kouremeti, Natalia
    • Atmospheric Measurement Techniques, Vol. 9, Issue 12
    • DOI: 10.5194/amt-9-5997-2016

    Brown carbon in the continental outflow to the North Indian Ocean
    journal, January 2019

    • Bikkina, Srinivas; Sarin, Manmohan
    • Environmental Science: Processes & Impacts, Vol. 21, Issue 6
    • DOI: 10.1039/c9em00089e

    Quantifying black carbon light absorption enhancement with a novel statistical approach
    journal, January 2018

    • Wu, Cheng; Wu, Dui; Yu, Jian Zhen
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 1
    • DOI: 10.5194/acp-18-289-2018

    Deriving brown carbon from multiwavelength absorption measurements: method and application to AERONET and Aethalometer observations
    journal, January 2016

    • Wang, Xuan; Heald, Colette L.; Sedlacek, Arthur J.
    • Atmospheric Chemistry and Physics, Vol. 16, Issue 19
    • DOI: 10.5194/acp-16-12733-2016

    Modeling the aging process of black carbon during atmospheric transport using a new approach: a case study in Beijing
    journal, January 2019

    • Zhang, Yuxuan; Li, Meng; Cheng, Yafang
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 14
    • DOI: 10.5194/acp-19-9663-2019

    Sulfate alters aerosol absorption properties in East Asian outflow
    journal, March 2018

    Optical properties of atmospheric fine particles near Beijing during the HOPE-J3A campaign
    journal, January 2016

    • Xu, Xuezhe; Zhao, Weixiong; Zhang, Qilei
    • Atmospheric Chemistry and Physics, Vol. 16, Issue 10
    • DOI: 10.5194/acp-16-6421-2016

    Amplification of light absorption of black carbon associated with air pollution
    journal, January 2018

    • Zhang, Yuxuan; Zhang, Qiang; Cheng, Yafang
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 13
    • DOI: 10.5194/acp-18-9879-2018

    An inter-comparison of black-carbon-related instruments in a laboratory study of biomass burning aerosol
    journal, October 2018

    Jury is still out on the radiative forcing by black carbon
    journal, August 2016

    • Boucher, Olivier; Balkanski, Yves; Hodnebrog, Øivind
    • Proceedings of the National Academy of Sciences, Vol. 113, Issue 35
    • DOI: 10.1073/pnas.1607005113

    Black carbon absorption at the global scale is affected by particle-scale diversity in composition
    journal, September 2016

    • Fierce, Laura; Bond, Tami C.; Bauer, Susanne E.
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms12361

    Biogenic and anthropogenic sources of aerosols at the High Arctic site Villum Research Station
    journal, January 2019

    • Nielsen, Ingeborg E.; Skov, Henrik; Massling, Andreas
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 15
    • DOI: 10.5194/acp-19-10239-2019

    Radiative Properties of Atmospheric Black Carbon (Soot) Particles with Complex Structures
    book, June 2019

    • He, Cenlin; Kokhanovsky, Alexander
    • Springer Series in Light Scattering: Volume 4: Light Scattering and Radiative Transfer, p. 219-254
    • DOI: 10.1007/978-3-030-20587-4_5

    Biomass-burning-derived particles from a wide variety of fuels – Part 1: Properties of primary particles
    journal, January 2020

    • McClure, Crystal D.; Lim, Christopher Y.; Hagan, David H.
    • Atmospheric Chemistry and Physics, Vol. 20, Issue 3
    • DOI: 10.5194/acp-20-1531-2020

    Black carbon absorption at the global scale is affected by particle-scale diversity in composition
    journal, September 2016

    • Fierce, Laura; Bond, Tami C.; Bauer, Susanne E.
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms12361

    The colors of biomass burning aerosols in the atmosphere
    journal, June 2016

    • Liu, Chao; Chung, Chul Eddy; Zhang, Feng
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep28267

    A Review of the Representation of Aerosol Mixing State in Atmospheric Models
    journal, March 2019

    Aerosol absorption retrieval at ultraviolet wavelengths in a complex environment
    journal, August 2016

    • Kazadzis, Stelios; Raptis, Panagiotis I.; Kouremeti, Natalia
    • Atmospheric Measurement Techniques Discussions
    • DOI: 10.5194/amt-2016-273

    Investigation of the absorption Ångström exponent and its relation to physicochemical properties for mini-CAST soot
    journal, April 2018

    Ageing and hygroscopicity variation of black carbon particles in Beijing measured by a quasi-atmospheric aerosol evolution study (QUALITY) chamber
    journal, January 2017

    On the accuracy of aerosol photoacoustic spectrometer calibrations using absorption by ozone
    journal, January 2018

    • Davies, Nicholas W.; Cotterell, Michael I.; Fox, Cathryn
    • Atmospheric Measurement Techniques, Vol. 11, Issue 4
    • DOI: 10.5194/amt-11-2313-2018

    Production of particulate brown carbon during atmospheric aging of residential wood-burning emissions
    text, January 2018

    Effects of mixing state on optical and radiative properties of black carbon in the European Arctic
    journal, January 2018

    • Zanatta, Marco; Laj, Paolo; Gysel, Martin
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 19
    • DOI: 10.5194/acp-18-14037-2018

    Effects of photochemical oxidation on the mixing state and light absorption of black carbon in the urban atmosphere of China
    journal, April 2017

    • Wang, Qiyuan; Huang, Rujin; Zhao, Zhuzi
    • Environmental Research Letters, Vol. 12, Issue 4
    • DOI: 10.1088/1748-9326/aa64ea

    Evidence in biomass burning smoke for a light-absorbing aerosol with properties intermediate between brown and black carbon
    journal, May 2019

    Vertical characterization of aerosol optical properties and brown carbon in winter in urban Beijing, China
    journal, January 2019

    • Xie, Conghui; Xu, Weiqi; Wang, Junfeng
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 1
    • DOI: 10.5194/acp-19-165-2019

    Simultaneous transmission and absorption photometry of carbon-black absorption from drop-cast particle-laden filters
    journal, March 2019

    Fine Particle Emissions from Sauna Stoves: Effects of Combustion Appliance and Fuel, and Implications for the Finnish Emission Inventory
    journal, December 2019

    • Tissari, Jarkko; Väätäinen, Sampsa; Leskinen, Jani
    • Atmosphere, Vol. 10, Issue 12
    • DOI: 10.3390/atmos10120775

    Emission factors and light absorption properties of brown carbon from household coal combustion in China
    journal, January 2017

    • Sun, Jianzhong; Zhi, Guorui; Hitzenberger, Regina
    • Atmospheric Chemistry and Physics, Vol. 17, Issue 7
    • DOI: 10.5194/acp-17-4769-2017

    Optical properties of atmospheric fine particles near Beijing during the HOPE-J3A Campaign
    journal, November 2015

    Effects of brown coatings on the absorption enhancement of black carbon: a numerical investigation
    journal, June 2018

    • Luo, Jie; Zhang, Yongming; Wang, Feng
    • Atmospheric Chemistry and Physics Discussions
    • DOI: 10.5194/acp-2018-600

    Quantification of online removal of refractory black carbon using laser-induced incandescence in the single particle soot photometer
    journal, April 2016

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