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Molecular Physics
An International Journal at the Interface Between Chemistry and Physics
Volume 73, 1991 - Issue 6
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Original Articles

Theory of rotational line strengths in coherent anti-Stokes Raman spectroscopy

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Pages 1257-1293 | Received 23 Nov 1990, Accepted 25 Feb 1991, Published online: 26 Oct 2007
 

Abstract

The general expressions for rotationally resolved CARS transitions involving molecular electronic states of arbitrary electronic angular momentum and spin are derived. All possible types of resonances (triple, double, Raman) are considered and the explicit results are presented for Hund's coupling cases (a) and (b) and intermediate (a–b) coupling. The results given are applicable to arbitrary incident laser polarizations. Calculations of practical interest are performed for three diatomics, namely OH, C2 and CH, for the triple resonance. Complete sets of closed formulae are tabulated for Hund's cases (a) and (b) for 3Π ← 3Π and 2Σ ← 2Π type transitions. With minor modifications, these expressions are also applicable to resonant degenerate four wave mixing.

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