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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Solvent effects over optical properties of a two-level molecular system

José Luis Paz, M. Gorayeb, A. J. Hernández

Published Oct 21, 2004• 0 citations
Publisher

Abstract

The solvent effects over optical properties of a two level system in presence of an electromagnetic field was modeled in this work. The system-field interaction was considered by using the dipolar-electric approximation, assuming negligible the molecular permanent dipole moments. The solvent effects were included in the formalism in a stochastic form, through the induced shifts over the Bohr molecular frequency. The coherence was calculated from the optical stochastic Bloch equations (OSBE), and later, it was averaged over all realizations of the stochastic molecular variable. To do that, it was applied the convolution theorem, which was resolved using direct and inverse Fourier transforms.

DOI
10.1117/12.590726

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The solvent effects over optical properties of a two level system in presence of an electromagnetic field was modeled in this work. The system-field interaction was considered by using the dipolar-electric approximation, assuming negligible the molecular permanent dipole moments. The solvent effects were included in the formalism in a stochastic form, through the induced shifts over the Bohr molecular frequency. The coherence was calculated from the optical stochastic Bloch equations (OSBE), and later, it was averaged over all realizations of the stochastic molecular variable. To do that, it was applied the convolution theorem, which was resolved using direct and inverse Fourier transforms.
The inclusion of the permanent dipole moments and the solvent on the optical conventional Bloch equations (OCBE) allowed us to obtain analytical expressions for the optical properties of a two-level molecular system. We employed the methodology developed by Colmenares et al.1, in which they model the collisional effect of the solvent through a stochastical function, ξ(t) = ω0 + σ(t), so the OCBE become a set of coupled integro-differential stochastical equations that we solved, up to third order in the incident field, employing the perturbation theory. Once obtained the analytical expressions for the density matrix elements, macroscopic polarization and effective susceptibility of the system, we studied the optical properties derived in the frequency space, inside and outside the rotating wave approximation.
Absorptive and dispersive nonlinear optical properties have been studied considering a two-level molecular system with permanent dipole moments immersed in a thermal reservoir interacting with a classical electromagnetic field. Our model is based in a stochastic description, where the system–solvent interaction induces random shifts in the Bohr frequency (ω0) that transforms ω0 into a stochastic variable ξ(t). Our results show that it is necessary to neglect the rotating-wave approximation in order to measure the effect of the permanent dipole moments. The two-photon transitions over those with one-photon are favored when the permanent dipole moments are considered.
The optical properties of a two-level molecular system immersed in a thermal reservoir and irradiated by an electromagnetic field were studied using the optical stochastic Bloch equations. The effect of the solvent is modeled as a stochastical shift of the system's Bohr frequency and the electromagnetic field includes both pump and probe fields. The resulting analytical expressions were studied by means of two and three dimensional graphics of the optical properties as a function of the pump-frequency detuning factor and the strength of the noise source.
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.
It was studied the solvent influence over a two level system interacting with an electromagnetic field using an stochastic treatment. It was considered a high-intensity electromagnetic field which is capable to produce local saturations. The induced coherence in the two electronic states, was averaged in the usual form, through both, Lorentzian and Gaussian probability density. From that, analytical expressions for susceptibility and optical properties were obtained. Numerical calculations were carried out to construct surfaces corresponding to this properties as a function of the field variables and the distributions parameters.
"Higher order effects of the electric field on the optical susceptibilities of a molecular system immersed in a thermal bath is studied in the present work. The molecule is viewed as a two level system, whose Bohr frequency is shifted randomly due to the interaction with the solvent. The optical Bloch equations were solved using the perturbation expantion of the field, and we have averaged over all realizations of the stochastic variable using gaussian and lorentzian distributions. Analytical expressions to the optical susceptibilities were found, which incorporte molecular and noise parameters. Susceptibilities surfaces are obtained as a fucntion of the detuning factor and the perturbation field."