Repository logo

Infoscience

  • English
  • French
Log In
Logo EPFL, École polytechnique fédérale de Lausanne

Infoscience

  • English
  • French
Log In
  1. Home
  2. Academic and Research Output
  3. Journal articles
  4. Atmospheric evolution of molecular-weight-separated brown carbon from biomass burning
 
research article

Atmospheric evolution of molecular-weight-separated brown carbon from biomass burning

Wong, Jenny P. S.
•
Tsagkaraki, Maria
•
Tsiodra, Irini
Show more
June 4, 2019
Atmospheric Chemistry And Physics

Biomass burning is a major source of atmospheric brown carbon (BrC), and through its absorption of UV/VIS radiation, it can play an important role in the planetary radiative balance and atmospheric photochemistry. The considerable uncertainty of BrC impacts is associated with its poorly constrained sources, transformations, and atmospheric lifetime. Here we report laboratory experiments that examined changes in the optical properties of the water-soluble (WS) BrC fraction of laboratory-generated biomass burning particles from hardwood pyrolysis. Effects of direct UVB photolysis and OH oxidation in the aqueous phase on molecular-weight-separated BrC were studied. Results indicated that the majority of low-molecular-weight (MW) BrC ( < 400 Da) was rapidly photobleached by both direct photolysis and OH oxidation on an atmospheric timescale of approximately 1 h. High MW BrC ( >= 400 Da) underwent initial photoenhancement up to similar to 15 h, followed by slow photobleaching over similar to 10 h. The laboratory experiments were supported by observations from ambient BrC samples that were collected during the fire seasons in Greece. These samples, containing freshly emitted to aged biomass burning aerosol, were analyzed for both water- and methanol-soluble BrC. Consistent with the laboratory experiments, high-MW BrC dominated the total light absorption at 365 nm for both methanol and water-soluble fractions of ambient samples with atmospheric transport times of 1 to 68 h. These ambient observations indicate that overall, biomass burning BrC across all molecular weights has an atmospheric lifetime of 15 to 28 h, consistent with estimates from previous field studies - although the BrC associated with the high-MW fraction remains relatively stable and is responsible for light absorption properties of BrC throughout most of its atmospheric lifetime. For ambient samples of aged (> 10 h) biomass burning emissions, poor linear correlations were found between light absorptivity and levoglucosan, consistent with other studies suggesting a short atmospheric lifetime for levoglucosan. However, a much stronger correlation between light absorptivity and total hydrous sugars was observed, suggesting that they may serve as more robust tracers for aged biomass burning emissions. Overall, the results from this study suggest that robust model estimates of BrC radiative impacts require consideration of the atmospheric aging of BrC and the stability of high-MW BrC.

  • Files
  • Details
  • Metrics
Type
research article
DOI
10.5194/acp-19-7319-2019
Web of Science ID

WOS:000470323500002

Author(s)
Wong, Jenny P. S.
Tsagkaraki, Maria
Tsiodra, Irini
Mihalopoulos, Nikolaos
Violaki, Kalliopi  
Kanakidou, Maria
Sciare, Jean
Nenes, Athanasios  
Weber, Rodney J.
Date Issued

2019-06-04

Publisher

Copernicus GmbH

Published in
Atmospheric Chemistry And Physics
Volume

19

Issue

11

Start page

7319

End page

7334

Subjects

Environmental Sciences

•

Meteorology & Atmospheric Sciences

•

Environmental Sciences & Ecology

•

humic-like substances

•

secondary organic aerosol

•

light-absorption

•

black carbon

•

observational constraints

•

hydroxyl radicals

•

oh oxidation

•

levoglucosan

•

chemistry

•

kinetics

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LAPI  
Available on Infoscience
June 21, 2019
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/158348
Logo EPFL, École polytechnique fédérale de Lausanne
  • Contact
  • infoscience@epfl.ch

  • Follow us on Facebook
  • Follow us on Instagram
  • Follow us on LinkedIn
  • Follow us on X
  • Follow us on Youtube
AccessibilityLegal noticePrivacy policyCookie settingsEnd User AgreementGet helpFeedback

Infoscience is a service managed and provided by the Library and IT Services of EPFL. © EPFL, tous droits réservés