Authors

Alicia Mullaley

Type

Text

Type

Dissertation

Advisor

Knopf, Daniel | Hameed, Sultan | Black, David | Zhang, Minghua | Fain, Xavier.

Date

2016-12-01

Keywords

Atmospheric chemistry -- Atmospheric sciences --

Department

Department of Marine and Atmospheric Science

Language

en_US

Source

This work is sponsored by the Stony Brook University Graduate School in compliance with the requirements for completion of degree.

Identifier

http://hdl.handle.net/11401/77760

Publisher

The Graduate School, Stony Brook University: Stony Brook, NY.

Format

application/pdf

Abstract

Carbon monoxide (CO) is a trace gas that influences atmospheric chemical reactions. CO is relatively short-lived (weeks to months) in the atmosphere and therefore spatially variable with a modern concentration range from 35 parts per billion (ppb) to 150 ppb (Globalview-CO, 2009). Because of its lifetime, atmospheric carbon monoxide is a good tracer for hemispheric processes; it is long enough to be transported over hemispheric distances but is short enough where there can be large seasonal and interannual variations. Therefore, measuring the variations in CO from bubbles trapped in Antarctic ice can reveal processes that occur in the Southern Hemisphere (SH). CO is the principal sink for the hydroxyl radical (OH) which is the most important oxidant in the atmosphere. The abundance of atmospheric OH can impact the lifetime of various atmospheric constituents such as the greenhouse gas methane (CH4), hydrofluorocarbons (HCFCs), non-methane hydrocarbons (NMHCs) and tropospheric ozone. In particular, because CO is the main loss mechanism for OH, increased concentrations of CO can cause a build-up of methane therefore affecting the global radiative budget and thus Earth’s climate. Once CO concentration is determined, the isotopes of CO provide valuable information on the source of CO. These new data will better constrain the sources and sinks of CO and thus its global cycle, helping to resolve uncertainties in climate models by providing additional constraints. Here I present a detailed investigation to determine atmospheric [CO] and stable CO isotopes 13CO and C18O from 1950 -1700 AD as recorded in bubbles trapped in ice cores from West Antarctic Ice Sheet Divide (WAIS D), Antarctica. This study better constrains the sources of atmospheric CO in the Southern Hemisphere during the late Holocene, including the contribution from biomass burning. The relationship between CO and CH4 over this time period is constructed based on these new observations and previously published CH4 paleo data. Overall, the results obtained from this study improve our understanding of the temporally varying sources of CO and the overall stability of tropospheric chemistry with respect to the CH4-CO-OH cycle. | Carbon monoxide (CO) is a trace gas that influences atmospheric chemical reactions. CO is relatively short-lived (weeks to months) in the atmosphere and therefore spatially variable with a modern concentration range from 35 parts per billion (ppb) to 150 ppb (Globalview-CO, 2009). Because of its lifetime, atmospheric carbon monoxide is a good tracer for hemispheric processes; it is long enough to be transported over hemispheric distances but is short enough where there can be large seasonal and interannual variations. Therefore, measuring the variations in CO from bubbles trapped in Antarctic ice can reveal processes that occur in the Southern Hemisphere (SH). CO is the principal sink for the hydroxyl radical (OH) which is the most important oxidant in the atmosphere. The abundance of atmospheric OH can impact the lifetime of various atmospheric constituents such as the greenhouse gas methane (CH4), hydrofluorocarbons (HCFCs), non-methane hydrocarbons (NMHCs) and tropospheric ozone. In particular, because CO is the main loss mechanism for OH, increased concentrations of CO can cause a build-up of methane therefore affecting the global radiative budget and thus Earth’s climate. Once CO concentration is determined, the isotopes of CO provide valuable information on the source of CO. These new data will better constrain the sources and sinks of CO and thus its global cycle, helping to resolve uncertainties in climate models by providing additional constraints. Here I present a detailed investigation to determine atmospheric [CO] and stable CO isotopes 13CO and C18O from 1950 -1700 AD as recorded in bubbles trapped in ice cores from West Antarctic Ice Sheet Divide (WAIS D), Antarctica. This study better constrains the sources of atmospheric CO in the Southern Hemisphere during the late Holocene, including the contribution from biomass burning. The relationship between CO and CH4 over this time period is constructed based on these new observations and previously published CH4 paleo data. Overall, the results obtained from this study improve our understanding of the temporally varying sources of CO and the overall stability of tropospheric chemistry with respect to the CH4-CO-OH cycle. | 188 pages

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