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Journal of Modern Optics

Solvent influence on the nonlinear optical properties of molecular systems in the presence of degenerate and non-degenerate four-wave mixing

José Luis Paz, Adriana Mendoza‐Garcia

Published Nov 30, 2011• 4 citations
Publisher

Abstract

The nonlinear optical properties are studied theoretically of a molecular system immersed in a thermal bath and interacting with a four-wave mixing signal. A methodology based on cumulant expansions to obtain the average in the Fourier components associated with the coherences and populations, calculated by the optical stochastic Bloch equations, is employed. The system properties are analyzed as a function of the frequency detuning of the high-intensity pump beam and parameterized by the frequency detuning of the probe beam, both with respect to the Bohr frequency of the system. The longitudinal and transversal relaxation times and the bath effects, modeled as white noise, are also included as parameters in the calculation. Different cases, with degenerate and non-degenerate optical frequencies are examined and compared, resulting in differences related to the maximum in the population pulsation effects.

DOI
10.1080/09500340.2011.639962

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The study of a two-level molecular system with permanent dipole moments (PDM) immersed in a thermal bath and interacting with an electromagnetic field depends on the inclusion of the rotating wave approximation (RWA). A methodology based on cumulant expansions to obtain the average in the Fourier components associated with the coherences and populations, calculated by the optical stochastic Bloch equations, is employed. With these equations, we have modeled the optical responses for the four-wave mixing signal and we have demonstrated that inside the RWA the PDM cannot be measured.
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.
We study the nonlinear absorptive and dispersive optical properties of molecular systems immersed in a thermal reservoir interacting with a four-wave mixing (FWM) signal. Residual spin-orbit Hamiltonians are considered in order to take into account the internal structure of the molecule. As system parameters in the dissipation processes, transverse and longitudinal relaxation times are considered for stochastic solute–solvent interaction processes. The intramolecular coupling effects on the optical responses are studied using a molecule model consisting of two coupled harmonic curves of electronic energies with displaced minima in nuclear energies and positions. In this study, the complete frequency space is considered through the pump–probe detuning, without restricting the derivations to only maximums of population oscillations. This approach opens the possibility of studying the behavior of optical responses, which is very useful in experimental design. Our results indicate the sensitivity of the optical responses to parameters of the molecular structure as well as to those derived from the photonic process of FWM signal generation.
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.
In this work we 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. Taking into account that the solvent produces an inhomogeneous displacement of the Bohr frequency and, employing a cumulant expansion to solve the stochastical equations derived, we obtained the mean values of the coherence, populations and susceptibilities Fourier components of the molecular system, from the optical stochastical Bloch equations (OSBE). These symmetry properties are used to show the dependence of the spectra with the frequency shifts of the incident fields, and we obtained 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 absence of the bath.