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Theory of pump-probe and four-wave mixing spectroscopy

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Abstract

In this paper we present theoretical calculations relating to pump-probe and four-wave mixing spectroscopy. In pump-probe spectroscopy, one measures the absorption profile for the situation when an arbitrary strong pump field drives a given transition and a probe (weak) field drives the same transition. We have studied the influence of level degeneracy and field polarization on pump-probe and four-wave mixing signals. Our results indicate that for some closed systems (no population loss to the reservoir) it is possible to observe resonances that are characterized by the ground state width. Previous calculations indicate that for a nondegenerate system this resonance can appear only for an open system, the so-called "pressure induced resonances.”1 Our result, which contradicts this conclusion, can be understood by noting the fact that there are in general three irreducible tensor2 (in general) contributions to the line shape (K = 0 population, K = 1 orientation, and K = 2 alignment). Thus, even if the system is closed for the population it may still remain open for orientation or alignment; this effect is responsible for the narrow resonance. Specific calculations are presented for J = 1/21/2 and J = 1→2 transitions.

© 1986 Optical Society of America

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