Exploring the observational constraints on the simulation of brown carbon

Wang, Xuan; Heald, Colette L.; Liu, Jiumeng; Weber, Rodney J.; Campuzano-Jost, Pedro; Jimenez, Jose L.; Schwarz, Joshua P.; Perring, Anne E.

doi:10.5194/acp-18-635-2018

Title: Exploring the observational constraints on the simulation of brown carbon

Journal Article · Fri Jan 19 00:00:00 EST 2018 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-18-635-2018· OSTI ID:1729864

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^[5]; Perring, Anne E. ^[6]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Harvard Univ., Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Univ. of Colorado, Boulder, CO (United States)
National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States)
Univ. of Colorado, Boulder, CO (United States); National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States)

Organic aerosols (OA) that strongly absorb solar radiation in the near-UV are referred to as brown carbon (BrC). The sources, evolution, and optical properties of BrC remain highly uncertain and contribute significantly to uncertainty in the estimate of the global direct radiative effect (DRE) of aerosols. Previous modeling studies of BrC optical properties and DRE have been unable to fully evaluate model performance due to the lack of direct measurements of BrC absorption. In this study, we develop a global model simulation (GEOS-Chem) of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental US (SEAC⁴RS and DC3). To the best of our knowledge, this is the first study to compare simulated BrC absorption with direct aircraft measurements. We show that BrC absorption properties estimated based on previous laboratory measurements agree with the aircraft measurements of freshly emitted BrC absorption but overestimate aged BrC absorption. In addition, applying a photochemical scheme to simulate bleaching/degradation of BrC improves model skill. The airborne observations are therefore consistent with a mass absorption coefficient (MAC) of freshly emitted biomass burning OA of 1.33 m² g^-1 at 365 nm coupled with a 1-day whitening e-folding time. Using the GEOS-Chem chemical transport model integrated with the RRTMG radiative transfer model, we estimate that the top-of-the-atmosphere all-sky direct radiative effect (DRE) of OA is -0.344 Wm^-2, 10 % higher than that without consideration of BrC absorption. Therefore, our best estimate of the absorption DRE of BrC is +0.048 Wm^-2. We suggest that the DRE of BrC has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USEPA; National Aeronautics and Space Administration (NASA)

Grant/Contract Number:: AC05-76RL01830; RD-83503301-0; NA16OAR4310112; NNX14AP74G; NNX15AT96G

OSTI ID:: 1729864

Report Number(s):: PNNL-SA-134105

Journal Information:: Atmospheric Chemistry and Physics (Online), Vol. 18, Issue 2; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Organic coating on sulfate and soot particles during late summer in the Svalbard Archipelago Yu, Hua; Li, Weijun; Zhang, Yangmei Atmospheric Chemistry and Physics, Vol. 19, Issue 15 https://doi.org/10.5194/acp-19-10433-2019	journal	January 2019
Photomineralization mechanism changes the ability of dissolved organic matter to activate cloud droplets and to nucleate ice crystals Borduas-Dedekind, Nadine; Ossola, Rachele; David, Robert O. Atmospheric Chemistry and Physics, Vol. 19, Issue 19 https://doi.org/10.5194/acp-19-12397-2019	journal	January 2019
Modelling black carbon absorption of solar radiation: combining external and internal mixing assumptions Curci, Gabriele; Alyuz, Ummugulsum; Barò, Rocio Atmospheric Chemistry and Physics, Vol. 19, Issue 1 https://doi.org/10.5194/acp-19-181-2019	journal	January 2019
Measuring light absorption by freshly emitted organic aerosols: optical artifacts in traditional solvent-extraction-based methods Shetty, Nishit J.; Pandey, Apoorva; Baker, Stephen Atmospheric Chemistry and Physics, Vol. 19, Issue 13 https://doi.org/10.5194/acp-19-8817-2019	journal	January 2019
Using CESM-RESFire to understand climate–fire–ecosystem interactions and the implications for decadal climate variability Zou, Yufei; Wang, Yuhang; Qian, Yun Atmospheric Chemistry and Physics, Vol. 20, Issue 2 https://doi.org/10.5194/acp-20-995-2020	journal	January 2020
Atmospheric evolution of molecular-weight-separated brown carbon from biomass burning Wong, Jenny P. S.; Tsagkaraki, Maria; Tsiodra, Irini Atmospheric Chemistry and Physics, Vol. 19, Issue 11 https://doi.org/10.5194/acp-19-7319-2019	journal	January 2019
Evaluating biases in filter-based aerosol absorption measurements using photoacoustic spectroscopy Davies, Nicholas W.; Fox, Cathryn; Szpek, Kate Atmospheric Measurement Techniques, Vol. 12, Issue 6 https://doi.org/10.5194/amt-12-3417-2019	journal	January 2019
Effect of heterogeneous oxidative aging on light absorption by biomass burning organic aerosol Browne, Eleanor C.; Zhang, Xiaolu; Franklin, Jonathan P. Taylor & Francis https://doi.org/10.6084/m9.figshare.7895765	text	January 2019
Effect of heterogeneous oxidative aging on light absorption by biomass burning organic aerosol Browne, Eleanor C.; Zhang, Xiaolu; Franklin, Jonathan P. Taylor & Francis https://doi.org/10.6084/m9.figshare.7895765.v2	text	January 2019
Modeling the global radiative effect of brown carbon: a potentially larger heating source in the tropical free troposphere than black carbon Zhang, Aoxing; Wang, Yuhang; Zhang, Yuzhong Atmospheric Chemistry and Physics, Vol. 20, Issue 4 https://doi.org/10.5194/acp-20-1901-2020	journal	January 2020
Biomass-burning-derived particles from a wide variety of fuels – Part 2: Effects of photochemical aging on particle optical and chemical properties Cappa, Christopher D.; Lim, Christopher Y.; Hagan, David H. Atmospheric Chemistry and Physics, Vol. 20, Issue 14 https://doi.org/10.5194/acp-20-8511-2020	journal	January 2020
Insights into the aging of biomass burning aerosol from satellite observations and 3D atmospheric modeling: evolution of the aerosol optical properties in Siberian wildfire plumes Konovalov, Igor B.; Golovushkin, Nikolai A.; Beekmann, Matthias Atmospheric Chemistry and Physics, Vol. 21, Issue 1 https://doi.org/10.5194/acp-21-357-2021	journal	January 2021

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