Date of Award

Spring 1-1-2011

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Atmospheric & Oceanic Sciences

First Advisor

Margaret A Tolbert

Second Advisor

O Brian Toon

Third Advisor

Weiqing Han

Abstract

Basic characteristics of the early Earth climate, the only known environment in the Universe in which life has been known to emerge and thrive, remain a mystery. In particular, little is understood about the Earth’s atmosphere 2.8 billion years ago. From climate models and laboratory studies, it is postulated that an organic haze, much like that found on Saturn’s largest moon Titan, covered the early Earth. This haze, generated from photolysis of carbon dioxide (CO2) and methane (CH4), may have had profound climatic consequences. Climate models of the early Earth that include this haze have had to rely upon optical properties of a Titan laboratory analog. Titan haze, though thought to be similar, is formed from a different combination of precursor gases and by different energy sources than early Earth haze.

This thesis examines the direct and indirect radiative effects of aerosol on early Earth climate by studying the optical and hygroscopic properties of a laboratory analog. A Titan analog is studied for comparison and to better understand spacecraft-retrieved haze chemical and optical properties from Titan. The properties of the laboratory analogs, generated in a flowing reactor cell with a continuum ultraviolet (UV) light source, were primarily measured using cavity ringdown aerosol extinction spectroscopy and UV-visible (UV-Vis) transmission spectroscopy.

We find that the optical properties of our early Earth analog are significantly different than those of the Titan analog from Khare et al. (1984). In both the UV and visible, when modeled as fractals, particles with the optical properties of the early Earth analog have approximately 30% larger extinction efficiencies than particles with Khare et al. (1984) values. This result implies our early Earth haze analog would provide a more efficient UV shield and have a stronger antigreenhouse effect than the Khare et al. (1984) Titan analog. Our Titan analog has significantly smaller imaginary refractive index values in the UV-Vis than Khare et al. (1984) values. These results may imply that (a) photolysis is not the dominant source of aerosol on Titan, and/or (b) the optical retrievals are dominated by the more absorbing and scattering electric discharge generated aerosol.

For the hygroscopicity studies, the optical growth of the early Earth analog at various relative humidities (RH) was measured, as well as a Titan analog for comparison. The retrieved hygroscopic parameter for the early Earth analog indicates that a humidified early Earth aerosol could have contributed to a larger antigreenhouse effect on the early Earth atmosphere than previously modeled with dry aerosol. Such effects would be important in regions where RH is greater than 50% because such high humidities are needed for significant amounts of water to be on the aerosol. The retrieved hygroscopicity parameter also indicates that the particles could activate into cloud droplets at reasonable supersaturations. In regions where the haze was dominant, it is expected that low particle concentrations, once activated into cloud droplets, would create short-lived, optically thin clouds. Such clouds, if predominant on the early Earth, would have a lower albedo than clouds today, thereby warming the planet relative to current day clouds.

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