Abstract

A method of calculation of nonlinear transient responses of an assembly of noninteracting polar linear molecules due to sudden changes in a strong external dc electric field is presented. The infinite hierarchy of differential-recurrence relations for the decay functions describing the relaxation of the system is derived by averaging the underlying inertial Langevin equation. The solution of this hierarchy is obtained in terms of matrix continued fractions. The integral relaxation time and the spectrum of the electric polarization for various nonlinear transient responses (step-on, step-off, and rapidly rotating field) are calculated for typical values of the model parameters. The nonlinear transient responses exhibit pronounced nonlinear effects due to the strong dc field. Analytical equations for the quantities of interest are presented in the overdamped limit. Furthermore, the linear response relaxation function and linear dynamic susceptibility are obtained as a particular case of a general nonlinear theory.

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