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Journal of Molecular Spectroscopy

A Formalism to Study the Propagation of the Four-Wave Mixing Signal in a Strongly Driven Two-Level System Immersed in a Thermal Reservoir

José Luis Paz, J. Récamier

Published Jun 1, 2000• 8 citations
Publisher
DOI
10.1006/jmsp.2000.8067

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This work studies the spatial propagation of the four-wave mixing signal of a molecular system with two electronic levels immersed in a thermal bath. Using the optical Bloch-Maxwell equations, we present three approximations, two of them are analytical solutions and the other is a numerical approach, where the effects of the variation of pump intensity through the optical path are considered. Also, we compare these results with the analogous in absence of the thermal reservoir and it is shown that the stochastic effect induced by the solvent, due to the experimental conditions as relaxation times, concentration of the solution and optical frequencies of the pumps, diminishes the intensity responses compared with the same in absence of the bath.
This work studies the spatial propagation of the Four-Wave Mixing (FWM) signal of a molecular system (malachite green) with two electronic levels immersed in a thermal bath, under a perturbative treatment at all order in the pump field and to first order in the probe and signal fields.Using the Optical Stochastic Bloch Equations OSBE, we present three approximations, two of them with analytical solutions and the third with a numerical approach, where the effects of the variation of pump intensity through the path optical are considered.We compare these results with the analogous in absence of the thermal reservoir.The stochastic effects induced by the solvent, due to the experimental conditions as relaxation times, chemical concentration of the solution and optical frequencies of the fields, diminishes the intensity responses compared with the same in absence of the bath.
Effects of spectral diffusion on the third-order nonlinear susceptibility for two- and three-level quantum systems, immersed in a thermal reservoir, are evaluated with a four-wave mixing (FWM) signal through the density matrix formalism. For this, inhomogeneously broadened two- and three-level quantum systems are used. In these models, the distribution of natural frequencies follows a Lorentzian function. The absorptive and dispersive nonlinear optical responses are determined for the considered quantum models. The results presented in this work show potential applications in the development of optical switches and provide a potential method to measure spectral diffusion relaxation times in three-level quantum systems.