Two-color resonant four-wave mixing: Analytical expressions for signal intensity

Journal Article · Sat Feb 01 04:00:00 EST 1997 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.473052· OSTI ID:450273

Williams, S; Rohlfing, E A; Rahn, L A ^[1]; Zare, R N ^[2]

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1. Combustion Research Facility, Sandia National Laboratories, Livermore, California 94551 (United States)
2. Department of Chemistry, Stanford University, Stanford, California 94305 (United States)

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. {bold 101}, 1072 (1994)] and TC-RFWM for the specific case of stimulated emission pumping [S. Williams {ital et al.}, J. Chem. Phys. {bold 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. {copyright} {ital 1997 American Institute of Physics.}

• OSTI ID: 450273
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 8 Vol. 106; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

40 CHEMISTRY
66 PHYSICS
ALIGNMENT
ANALYTICAL SOLUTION
DOUBLE RESONANCE METHODS
FREQUENCY MIXING
LINE WIDTHS
MOLECULES
ORIENTATION
PERTURBATION THEORY
SPECTROSCOPY
STIMULATED EMISSION