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Preprints
https://doi.org/10.5194/acp-2020-591
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-591
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 29 Jun 2020

Submitted as: research article | 29 Jun 2020

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This preprint is currently under review for the journal ACP.

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

Igor B. Konovalov1, Nikolai A. Golovushkin1, Matthias Beekmann2, and Meinrat O. Andreae3,4,5 Igor B. Konovalov et al.
  • 1Institute of Applied Physics, Russian Academy of Sciences, Nizhniy Novgorod, Russia
  • 2LISA/IPSL, Laboratoire Interuniversitaire des Systèmes Atmosphériques, UMR CNRS 7583, Université Paris Est Créteil (UPEC) et Université Paris Diderot (UPD), France
  • 3Max Planck Institute for Chemistry, Mainz, Germany
  • 4Scripps Institution of Oceanography, University of California San Diego, La Jolla, CA 92093, USA
  • 5Department of Geology and Geophysics, King Saud University, Riyadh, Saudi Arabia

Abstract. Long-range transport of biomass burning (BB) aerosol from regions affected by wildfires is known to have a significant impact on the radiative balance and air quality in receptor regions, including the Arctic. However, the atmospheric evolution of the optical properties of BB aerosol during the long-range transport events is insufficiently understood, limiting the adequacy of representations of the aerosol processes in chemistry transport and climate models. Here we introduce a framework to infer and interpret changes of the optical properties of BB aerosol from satellite observations of multiple BB plumes. Our framework includes (1) a procedure for analysis of available satellite retrievals of the absorption and extinction aerosol optical depths (AAOD and AOD) and single scattering albedo (SSA) as a function of the BB aerosol photochemical age, and (2) a representation of the AAOD and AOD evolution with a chemistry transport model (CTM) involving a simplified volatility basis set (VBS) scheme with a few adjustable parameters. We apply this framework to analyze a large-scale outflow of BB smoke plumes from Siberia toward Europe that occurred in July 2016. We use AAOD and SSA data derived from OMI (Ozone Monitoring Instrument) satellite measurements in the near-UV range along with 550 nm AOD and carbon monoxide (CO) columns retrieved from MODIS (Moderate Resolution Imaging Spectroradiometer) and IASI (Infrared Atmospheric Sounding Interferometer) satellite observations, respectively, to infer changes in the optical properties of Siberian BB aerosol due to its atmospheric aging and to get insights into the processes underlying these changes. Using the satellite data in combination with simulated data from the CHIMERE CTM, we evaluate the enhancement ratios (EnR) that allow isolating AAOD and AOD changes due to oxidation and gas-particle partitioning processes from those due to other processes, including transport, deposition, and wet scavenging. The behavior of EnRs for AAOD and AOD is then characterized using nonlinear trend analysis. It is found that the EnR for AOD strongly increases (by about a factor of 2) during the first 20–30 hours of the analyzed evolution period, whereas the EnR for AAOD does not exhibit a statistically significant increase during this period. The increase in AOD is accompanied by a statistically significant enhancement of SSA. Further BB aerosol aging (up to several days) is associated with a strong decrease of EnRs for both AAOD and AOD. Our simulations constrained by the observations indicate that the upward trends in EnR for AOD and in SSA are mainly due to atmospheric processing of secondary organic aerosol (SOA), leading to an increase in the mass scattering efficiency of BB aerosol. Evaporation and chemical fragmentation of the SOA species, part of which is assumed to be absorptive (to contain brown carbon), are identified as a likely reason for the subsequent decrease of the EnR for both AAOD and AOD. Hence, our analysis reveals that the long-range transport of smoke plumes from Siberian fires is associated with major changes in BB aerosol optical properties and chemical composition. Overall, this study demonstrates the feasibility of using available satellite observations for evaluating and improving representations in atmospheric models of the BB aerosol aging processes in different regions of the world at much larger temporal scales than those typically addressed in aerosol chamber experiments.

Igor B. Konovalov et al.

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Igor B. Konovalov et al.

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Latest update: 05 Jul 2020
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Short summary
A lack of consistent observational constraints on the atmospheric evolution of the optical properties of biomass burning (BB) aerosol limits the accuracy of assessments of the aerosol raditative and climate effects. We show that useful insights into the evolution of the BB aerosol optical properties can be inferred from a combination of satellite observations and 3D-modeling. Major changes in the BB aerosol optical properties are found to occur during the long-range transport of Siberian smoke.
A lack of consistent observational constraints on the atmospheric evolution of the optical...
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