Formation of ozone and growth of aerosols in young smoke plumes from biomass burning

The combustion of biomass is a major source of atmospheric trace gases and aerosols. Regional and global-scale models of atmospheric chemistry and climate take estimates for these emissions and arbitrarily "mix" them into grid boxes with horizontal scales of 10-200 km. This procedure ignores the complex non-linear chemical and physical transformations that take place in the highly concentrated environment of the young smoke plumes. In addition, the observations of the smoke plume from the Timbavati savannah fire [Hobbs et al., 2003] show much higher concentrations of ozone and secondary aerosol matter (nitrate, sulfate, and organic carbon [OC]) in the smoke plume than are predicted by current atmospheric chemistry models. To address these issues, we developed a new model of the gas- and aerosol-phase chemistry of biomass burning smoke plumes called ASP (Aerosol Simulation Program). Here we use ASP to simulate the gas-phase chemistry and particle dynamics of young biomass burning smoke plumes and to estimate the errors introduced by the artificial mixing of biomass burning emissions into large-scale grid boxes. This work is the first known attempt to simultaneously simulate the dynamics, gas-phase chemistry, aerosol-phase chemistry, and radiative transfer in a young biomass burning smoke plume. We simulated smoke plumes from three fires using ASP combined with a Lagrangian parcel model. We found that our model explained the formation of ozone in the Otavi and Alaska plumes fairly well but that our initial model simulation of the Timbavati smoke plume underestimated the formation of ozone and secondary aerosol matter. The initial model simulation for Timbavati appears to be missing a source of OH. Heterogeneous reactions of NO2 and SO2 could explain the high concentrations of OH and the rapid formation of ozone, nitrate and sulfate in the smoke plume if the uptake coefficients on smoke aerosols are large [O(10-3) and O(10-4), respectively]. Uncharacterized organic species in the smoke plume were likely responsible for the rapid formation of aerosol OC. The changes in the aerosol size distribution in our model simulations were dominated by plume dilution and condensational growth, with coagulation and nucleation having only a minor effect.

Department dc:contributor.department

Massachusetts Institute of Technology. Dept. of Earth, Atmospheric, and Planetary Sciences.

Grantor dc:publisher

Massachusetts Institute of Technology

Year dc:date.issued

2008

Author dc:creator

• Alvarado, Matthew James

Advisor dc:contributor.advisor

• Ronald G. Prinn.

• Earth, Atmospheric, and Planetary Sciences.

Statement dc:rights

• M.I.T. theses are protected by copyright. They may be viewed from this source for any purpose, but reproduction or distribution in any format is prohibited without written permission. See provided URL for inquiries about permission.

Licence dc:rights.uri

• http://dspace.mit.edu/handle/1721.1/7582

Language dc:language.iso

eng

Handle dc:identifier.uri

http://hdl.handle.net/1721.1/45606

OAI identifier oai:identifier

oai:dspace.mit.edu:1721.1/45606