On the physical mechanisms of relaxation time distribution in disordered dielectrics

TL;DR

This paper models the distribution of relaxation times in disordered dielectrics using random field theory, revealing how nonlinear effects and spatial correlations influence relaxation behavior and phase coexistence.

Contribution

It provides a self-consistent calculation of relaxation time distribution considering nonlinear random fields and spatial correlations, linking theoretical models to empirical relaxation functions.

Findings

Nonlinear random fields cause asymmetric relaxation time distributions.

Relaxation functions correspond to a mixed ferro-glass phase.

Different empirical relaxation functions relate to linear or nonlinear random field contributions.

Abstract

The distribution function of relaxation times in disordered dielectrics has been calculated in the random field theory framework. For this purpose, we first consider the dynamics of single two-orientable impurity electric dipole in a random electric field $E$ created by the rest of impurities in disordered ferroelectric. This dynamics is conveniently described by Langevin equation. Relaxation time $\tau $ is then a reciprocal probability (calculated on the base of Fokker-Planck equation) of the dipole transition through barrier in a double-well potential (corresponding to two possible dipole orientations), distorted by a random fields. The obtained dependence $\tau (E)$ made it possible to obtain the expression for relaxation times distribution function $F(\tau)$(via random fields distribution function $f(E)$. Latter function has been calculated self-consistently in the random field theory framework. Nonlinear random field contribution and effects of spatial correlations between impurities have also been taken into account. It was shown that nonlinear contribution of random field gives asymmetric shape of $F(\tau)$, while in linear case it is symmetric. Comparison of calculated $F(\tau)$ curves with those extracted from empirical Cole-Cole (CC), Davidson-Cole (DC), Kohlrausch-William-Watts (KWW) and Havriliak-Negami (HN) functions had shown, that they correspond to mixed ferro-glass phase with coexistence of short and long-range order. Different forms of $F(\tau)$ are determined by linear (CC) or nonlinear (DC, KWW, HN) contributions of random field.