Final Report: Investigating the Effects Of Atmospheric Aging on the Radiative Properties and Climate Impacts of Black Carbon Aerosol

EPA Grant Number: R835033
Title: Investigating the Effects Of Atmospheric Aging on the Radiative Properties and Climate Impacts of Black Carbon Aerosol
Investigators: Kroll, Jesse H. , Davidovits, Paul , Heald, Colette L.
Institution: Massachusetts Institute of Technology , Boston College
EPA Project Officer: Hunt, Sherri
Project Period: May 1, 2012 through April 30, 2015 (Extended to April 30, 2016)
Project Amount: $899,654
RFA: Black Carbon's Role In Global To Local Scale Climate And Air Quality (2010) RFA Text |  Recipients Lists
Research Category: Global Climate Change , Climate Change , Air

Objective:

Black carbon (BC) particles play a significant role in climate forcing, yet the effects of aging—atmospheric processes that affect the mass, size, shape and chemical composition of aerosol particles—on their radiative properties are poorly constrained. The goal of this combined laboratory and modeling study was to provide new insights into the detailed effects of atmospheric aging on the climate impacts of black carbon particles.

Summary/Accomplishments (Outputs/Outcomes):

Laboratory experiments were focused on the atmospheric aging of BC particles, with initial studies examining how their chemical composition and water-uptake properties change as a result of the heterogeneous oxidation by OH or O3. This chemistry was shown to be driven by the oxidation of organics on the surface of the BC particles, a process that was found to occur on timescales similar to other aging processes (such as the condensation of secondary species). A large experimental intensive examined changes to optical properties (scattering and absorption) of BC particles upon condensation of secondary sulfate and organic aerosol, with analysis of results still ongoing. The formation and evolution of “brown carbon” (BrC, light-absorbing organic aerosol) was also examined, by measuring the optical properties of secondary organic aerosol (which under low-NOx conditions were shown to be only weakly absorbing) and examining how primary BrC (from biomass burning) evolves both chemically and optically. In this latter set of studies, it was found that heterogeneous oxidation clearly “whitens” the particles, suggesting a quite limited lifetime for atmospheric BrC, in agreement with recent fieldwork. In the modeling sphere, a radiative transfer model was integrated into the global chemical transport model GEOS-Chem, enabling determinations of direct radiative effects. This allowed for an exploration of the direct radiative effect and direct radiative forcing of aerosols in present-day and future emissions scenarios, and moreover improved estimates of the global climate impacts of BC. In particular, it was shown that climate forcing by black carbon is likely substantially lower than currently estimated. This work motivated additional work to explore the absorption from BrC, including one published study on the global observational constraints on BrC absorption and ongoing work to model the potential climate impacts of BrC. 


Journal Articles on this Report : 9 Displayed | Download in RIS Format

Other project views: All 25 publications 9 publications in selected types All 9 journal articles
Type Citation Project Document Sources
Journal Article Browne EC, Franklin JP, Canagaratna MR, Massoli P, Kirchstetter TW, Worsnop DR, Wilson KR, Kroll JH. Changes to the chemical composition of soot from heterogeneous oxidation reactions. Journal of Physical Chemistry A 2015;119(7):1154-1163. R835033 (2014)
R835033 (Final)
  • Abstract from PubMed
  • Full-text: ACS-Full Text PDF
    Exit
  • Abstract: ACS-Abstract
    Exit
  • Other: MIT-Full Text PDF
    Exit
  • Journal Article Canagaratna MR, Massoli P, Browne EC, Franklin JP, Wilson KR, Onasch TB, Kirchstetter TW, Fortner EC, Kolb CE, Jayne JT, Kroll JH, Worsnop DR. Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization. Journal of Physical Chemistry A 2015;119(19):4589-4599. R835033 (Final)
  • Abstract from PubMed
  • Full-text: ACS-Full Text HTML
    Exit
  • Abstract: ACS-Abstract
    Exit
  • Other: ACS-Full Text PDF
    Exit
  • Journal Article Heald CL, Ridley DA, Kroll JH, Barrett SRH, Cady-Pereira KE, Alvarado MJ, Holmes CD. Contrasting the direct radiative effect and direct radiative forcing of aerosols. Atmospheric Chemistry and Physics 2014;14(11):5513-5527. R835033 (2013)
    R835033 (2014)
    R835033 (Final)
  • Full-text: ACP-Full Text PDF
    Exit
  • Abstract: ACP-Abstract
    Exit
  • Other: ResearchGate-Full Text PDF
    Exit
  • Journal Article Lambe AT, Cappa CD, Massoli P, Onasch TB, Forestieri SD, Martin AT, Cummings MJ, Croasdale DR, Brune WH, Worsnop DR, Davidovits P. Relationship between oxidation level and optical properties of secondary organic aerosol. Environmental Science & Technology 2013;47(12):6349-6357. R835033 (2012)
    R835033 (2013)
    R835033 (2014)
    R835033 (Final)
  • Abstract from PubMed
  • Full-text: ACPD-Full Text PDF
    Exit
  • Abstract: ES&T-Abstract
    Exit
  • Journal Article Lambe AT, Ahern AT, Wright JP, Croasdale DR, Davidovits P, Onasch TB. Oxidative aging and cloud condensation nuclei activation of laboratory combustion soot. Journal of Aerosol Science 2015;79:31-39. R835033 (2014)
    R835033 (Final)
  • Full-text: ScienceDirect-Full Text HTML
    Exit
  • Abstract: ScienceDirect-Abstract
    Exit
  • Other: ScienceDirect-Full Text PDF
    Exit
  • Journal Article Onasch TB, Fortner EC, Trimborn AM, Lambe AT, Tiwari AJ, Marr LC, Corbin JC, Mensah AA, Williams LR, Davidovits P, Worsnop DR. Investigations of SP-AMS carbon ion distributions as a function of refractory black carbon particle type. Aerosol Science and Technology 2015;49(6):409-422. R835033 (2014)
    R835033 (Final)
    R833747 (Final)
  • Full-text: Taylor & Francis-Full Text PDF
    Exit
  • Abstract: Taylor & Francis-Abstract & Full Text HTML
    Exit
  • Journal Article Sedlacek III AJ, Lewis ER, Onasch TB, Lambe AT, Davidovits P. Investigation of refractory black carbon-containing particle morphologies using the Single-Particle Soot Photometer (SP2). Aerosol Science and Technology 2015;49(10):872-885. R835033 (2014)
    R835033 (Final)
  • Full-text: Taylor & Francis-Full Text HTML
    Exit
  • Abstract: Taylor & Francis-Abstract
    Exit
  • Other: Taylor & Francis-Full Text PDF
    Exit
  • Journal Article Wang X, Heald CL, Ridley DA, Schwarz JP, Spackman JR, Perring AE, Coe H, Liu D, Clarke AD. Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon. Atmospheric Chemistry and Physics 2014;14(20):10989-11010. R835033 (2014)
    R835033 (Final)
  • Full-text: ACP-Full Text PDF
    Exit
  • Abstract: ACP-Abstract
    Exit
  • Journal Article Wang X, Heald CL, Sedlacek AJ, de Sa SS, Martin ST, Alexander ML, Watson TB, Aiken AC, Springston SR, Artaxo P. Deriving brown carbon from multiwavelength absorption measurements:method and application to AERONET and Aethalometer observations. Atmospheric Chemistry and Physics 2016;16(19):12733-12752. R835033 (Final)
  • Full-text: ACP-Full Text PDF
    Exit
  • Abstract: ACP-Abstract
    Exit
  • Supplemental Keywords:

    Aerosol, atmospheric aging, black carbon, brown carbon, climate, direct radiative effects, global modeling, light-absorbing carbon, optical properties

    Progress and Final Reports:

    Original Abstract
    2012 Progress Report
    2013 Progress Report
    2014 Progress Report