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Journal of Nonlinear Optical Physics & Materials

SOLVENT COLLISIONAL EFFECTS IN FOUR-WAVE MIXING

A. Mastrodoménico, M. A. IZQUIERDO, José Luis Paz

Published Jun 1, 2012• 3 citations
Publisher

Abstract

The stochastic effects of a thermal bath on a two-level molecular system interacting with a classical electromagnetic field are considered. The collective effects are modeled as a random Bohr frequency, whose manifestation is the broadening of the upper level according to a prescribed random function. A methodology based in cumulant expansions to obtain the average in the Fourier components associated with the coherence and populations, calculated by Optical Stochastic Bloch Equations (OSBE), is employed. The Four-wave mixing signal intensity as a function of the detuning of the pump beam, parametrized by the ratio of the relaxation times and other variables, is analyzed.

DOI
10.1142/s0218863512500166

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In this work are studied the symmetry properties of the Rayleigh-type optical mixing signal of a two-level molecular system immersed in a thermal bath and irradiated by a classical electromagnetic field. The solvent induces a random shift of the Bohr frequency in the molecular system. A methodology based in cumulant expansions is employed to obtain the average of the coherences, populations, and susceptibilities of Fourier components associated, calculated by the optical stochastic Bloch equations. These symmetry properties show the dependence of the measured spectra with the variations in the frequencies of the incident fields. Our results show that the inclusion of the thermal bath diminishes the intensity response as well it promotes the loss of the symmetry properties, compared with the same results in the 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.