Abstract
We present analytical signal expressions for each two-color resonant four-wave mixing (TC-RFWM) scheme that can be used for double-resonance molecular spectroscopy in the limit of weak fields (no saturation). The theoretical approach employs time-independent, diagrammatic perturbation theory and a spherical tensor analysis in an extension of recent treatments of degenerate four-wave mixing [S. Williams, R. N. Zare, and L. A. Rahn, J. Chem. Phys. 101, 1072 (1994)] and TC-RFWM for the specific case of stimulated emission pumping [S. Williams et al., J. Chem. Phys. 102, 8342 (1995)]. Under the assumption that the relaxation of the population, the orientation, and the alignment are the same, simple analytic expressions are derived for commonly used experimental configurations. The TC-RFWM signal is found to be a product of a concentration term, a one-photon molecular term, a line shape function, and a laboratory-frame geometric factor. These expressions are intended to facilitate the practical analysis of TC-RFWM spectra by clarifying, for example, the dependence on beam polarizations and rotational branch combinations.
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