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ROTATIONALLY RESOLVED $\tilde{A}^2$A$_1$ - $\tilde{X}^2$E ELECTRONIC SPECTRA OF SYMMETRIC METHOXY RADICALS: CH$_3$O AND CD$_3$O

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Title: ROTATIONALLY RESOLVED $\tilde{A}^2$A$_1$ - $\tilde{X}^2$E ELECTRONIC SPECTRA OF SYMMETRIC METHOXY RADICALS: CH$_3$O AND CD$_3$O
Creators: Chen, Ming-Wei; Liu, Jinjun; Melnik, Dmitry G.; Miller, Terry A.
Issue Date: 2008
Abstract: Methoxy radical, a key component in both atmospheric and combustion chemistry, has attracted spectroscopic interest for more than twenty years. Microwave measurements of CH$_3$O}, \underline{\textbf{81}}, 122 (1984)}} and CD$_3$O}}} with precision on the kHz scale have determined the $\tilde{X}^2$E parameters. Jet-cooled laser induced fluorescence (LIF) spectra} {61$^{st}$ International Symposium on Molecular Spectroscopy, (2006)}} have also been observed by our group for both CH$_3$O and CD$_3$O, with high-resolution ($\Delta\nu\approx$250 MHz) and high-accuracy ($\Delta\sigma\approx$50 MHz), for the 3$^2_0$ and 6$^1_0$ bands of the $\tilde{A}^2$A$_1$ - $\tilde{X}^2$E$_{3/2}$ electronic transition. Since the ground state component E$_{1/2}$ is $\approx$60 cm$^{-1}$ energetically higher than the E$_{3/2}$ spin component, the $\tilde{X}^2$E$_{1/2}$ state is not thermally populated in a jet-cooled environment. However, our complementary stimulated emission pumping (SEP) experiment directly interrogates the $\tilde{X}^2$E$_{1/2}$ level of CH$_3$O and CD$_3$O by depleting the fluorescence from $\tilde{A}^2$A$_1$ 3$^2$ excited levels. It has now been performed with the same resolution and accuracy as the LIF work. The global analysis of the microwave$^{b,c}$, LIF, and SEP data breaks correlations in the microwave data and provides better determinations for the $\tilde{X}$ and $\tilde{A}$ states' parameters. Comparison of the values for CH$_3$O, $^{13}$CH$_3$O}, \underline{\textbf{88}}, 5338 (1988)}}, and CD$_3$O allows us to separate first-order from second-order electronic and vibrational contributions based upon the isotopic dependencies of the effective ground state parameters, \textit{e.g.} the Jahn-Teller parameters \textit{h$_1$} and \textit{h$_2$}, spin-rotation parameters, etc.
URI: http://hdl.handle.net/1811/33583
Other Identifiers: 2008-RI-08
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