Nonlinear response theory for Markov processes. II. Fifth-order response functions. 2017

Gregor Diezemann
Institut für Physikalische Chemie, Universität Mainz, Duesbergweg 10-14, 55128 Mainz, Germany.

The nonlinear response of stochastic models obeying a master equation is calculated up to fifth order in the external field, thus extending the third-order results obtained earlier [G. Diezemann, Phys. Rev. E 85, 051502 (2012)PLEEE81539-375510.1103/PhysRevE.85.051502]. For sinusoidal fields the 5ω component of the susceptibility is computed for the model of dipole reorientations in an asymmetric double well potential and for a trap model with a Gaussian density of states. For most realizations of the models a hump is found in the higher-order susceptibilities. In particular, for the asymmetric double well potential model there are two characteristic temperature regimes showing the occurrence of such a hump as compared to a single characteristic regime in the case of the third-order response. In the case of the trap model the results strongly depend on the variable coupled to the field. As for the third-order response, the low-frequency limit of the susceptibility plays a crucial role with respect to the occurrence of a hump. The findings are discussed in light of recent experimental results obtained for supercooled liquids. The differences found for the third-order and the fifth-order response indicate that nonlinear response functions might serve as a powerful tool to discriminate among the large number of existing models for glassy relaxation.

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