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Inertia of the oscillatory mechanisms of giant nonlinearities of optical materials in the terahertz spectral range

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Abstract

Subject of study. The inertia of the oscillatory mechanisms of the nonlinearities of isotropic dielectric media in the field of the terahertz-frequency electromagnetic waves was investigated for resonant and nonresonant interactions between radiation and matter. The purpose of this work was to construct a dynamic model of the nonlinear polarization responses of optical media with oscillatory nature in the field of terahertz pulses and to estimate the time constants characterizing the inertia of such responses during resonant and nonresonant interactions between radiation and media molecular vibrations. Method. The model of anharmonic vibrations of the atoms of each molecule as an oscillator in the general case for an isotropic medium, with both quadratic and cubic nonlinearities, was reduced for a macroscopic optical characteristic—its polarization—to a model as a system of parametrically coupled equations with only cubic nonlinearities. The system parameters were determined from well-known characteristics of a medium, such as its thermal expansion coefficient, stretching molecular vibration frequency, and refractive index. Main results. Expressions were obtained for the inertial time constants of the cubic susceptibilities of optical media with nonlinear vibrations in two- and one-photon resonant interactions with quasi-monochromatic terahertz pulses as well as in nonresonant interactions with broadband terahertz pulsed radiation through the thermal, spectral, and optical characteristics of materials known in the literature. Numerical estimates were obtained for the inertial time constants of the nonlinear susceptibilities of media with particularly high vibrational nonlinearities in the refractive indices, namely, α-pinene and water, as well as silicon dioxide. For these materials, the inertial time constants of the resonant oscillatory mechanisms of the nonlinearities for radiation in the terahertz spectral range were shown to be of the order of hundreds of femtoseconds; for the nonresonant interactions, the time constants decreased to ten femtoseconds or less. Practical significance. The obtained inertial time constant estimations of the polarization responses of materials indicate that their giant nonlinearities in the far infrared spectral range could be used to develop ultrafast photonic devices for pulsed terahertz radiation parameter control.

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