SELECTIVE EXCITATION AND SPECTROSCOPY OF HIGH VIBRATIONAL LEVELS OF a1A1 CH2 BY STIMULATED EMISSION PUMPING

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1988

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Ohio State University

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Using stimulated emission pumping with two laser pulses, we have shown that high vibrational levels of a short-lived radical can be studied, and a large population can be prepared at a single, selected, high vibration-rotation level. The first demonstration was performed on the $\nu_{3}=3$ level of $a_{1}A_{1} CH_{2}$. The methylene radical was produced by photolysis of the ketene molecule. The pump laser pulse excites the $b \leftarrow a 2_{0}^{1}$ transition and the dump laser stimulates emission through the $a \leftarrow b, 2_{3}^{1}$ transitions. In addition to the determination of molecular constants, the double-resonance technique will enable us to determine whether the singlet-triplet coupling that prevails in the $a \leftarrow b$ transitions originates in the a or b state. The double minima in the bending potential can also be characterized.

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Author Institution: Chemistry Department, University of Pennsylvania Philadelphia

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