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

Study of the optical properties of a molecular system interacting with a high-intensity electromagnetic field

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

Published Oct 21, 2004• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.590734

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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.
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.
"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."
Analytic approximations for the absorption coefficient and refraction index have been obtained for a two-level molecular system in the presence of a four-wave mixing signal. Stochastic collisions among solute–solvent molecules produce a broadening of the upper level of energy. In this work, we have used four generalized Lorentzian approximants of the Voigt function as probability distribution, calculated by the two-point quasi-rational approximant method previously denoted as asymptotical Padé technique, for the evaluation of the average values of the Fourier components associated to the induced coherences. The innovation of this type of distributions allows us, by taking appropriate limits, to find similar profiles of optical properties as those using Gaussian and Lorentzian distribution functions.
In this work, the thermal reservoir effects over the absorptive and dispersive nonlinear optical properties of a two-level molecular system in presence of classical electromagnetic fields, were modeled. The collective effects proper of the thermal reservoir are modeled as a time dependent frequency, whose manifestation is the broadening of the upper level according to a prescribed random function. Using the stochastic optical Bloch equations, analytical expression for the nonlinear induced susceptibilities and absorptive and dispersive optical properties, were obtained. Numerical calculations were carried out to construct surfaces corresponding to these optical properties as a function of the pump-probe frequency detuning, relationships between the longitudinal and transversal relaxation times, and molecular concentration of solute. Finally, we see an attenuation of these optical responses by the solvent effects and the high pump-intensity.
It was studied the solvent influence over a two level system in the four wave mixing spectroscopy. the solvente effect was incorporated to the model in a stochastic form, through the broadening of the upper molecular level. Two intense waves of the same frequency, ω1, and another wave with minor intensity and ω2 frequency, were considered coupled to the nonlinear system, generating a new signal whose frequency is ω3, and where the wave-vectors follow the relation vector k1 + vector k1 = vector k2 + vector k3. Using the dipolar-electric and the rotating wave approximations, it was calculated the average of the coherence at the ω1, ω2 and ω3 frequencies. From that results, analytical expressions to the susceptibilities at the studied frequencies were obtained. Linear, coherent and coupled processes were identified.
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.