Onset of the nonlinear dielectric response of glasses in the two-level system model

TL;DR

This paper models the nonlinear dielectric response of glasses at low temperatures using a two-level system approach, revealing the importance of defect interactions and a new relaxation rate to match experimental data.

Contribution

It introduces a quantum simulation incorporating a new defect interaction relaxation rate that explains experimental nonlinear dielectric susceptibility data.

Findings

The standard two-level model predicts a decrease in susceptibility with increasing field, contrary to experiments.

Including a field-dependent relaxation rate aligns model predictions with experimental observations.

The new relaxation mechanism suggests testable effects in ultra-thin samples and on nonequilibrium behavior.

Abstract

We have calculated the real part $\chi'$ of the nonlinear dielectric susceptibility of amorphous insulators in the kHz range, by using the two-level system model and a nonperturbative numerical quantum approach. At low temperature $T$, it is first shown that the standard two-level model should lead to a \textit{decrease} of $\chi'$ when the measuring field $E$ is raised, since raising $E$ increases the population of the upper level and induces Rabi oscillations canceling the ones induced from the ground level. This predicted $E$-induced decrease of $\chi'$ is at \textit{odds} with experiments. However, a \textit{good agreement} with low-frequency experimental nonlinear data is achieved if, in our fully quantum simulations, interactions between defects are taken into account by a new relaxation rate whose efficiency increases as $\sqrt{E}$, as was proposed recently by Burin \textit{et al.} (Phys. Rev. Lett. {\bf 86}, 5616 (2001)). In this approach, the behavior of $\chi'$ at low $T$ is mainly explained by the efficiency of this new relaxation channel. This new relaxation rate could be further tested since it is shown that it should lead: \textit{i)} to a completely new nonlinear behavior for samples whose thickness is $\simeq 10$ nm; \textit{ii)} to a decrease of nonequilibrium effects when $E$ is increased.