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Linear response approximations are central to our understanding and simulations of nonequilibrium statistical mechanics. Despite the success of these approaches in predicting nonequilibrium dynamics, open questions remain. Laird and Thompson [J. Chem. Phys. 126, 211104 (2007)] previously formalized, in the context of solvation dynamics, the connection between the static linear-response approximation and the assumption of Gaussian statistics. The Gaussian statistics perspective is useful in understanding why linear response approximations are still accurate for perturbations much larger than thermal energies. In this paper, we use this approach to address three outstanding issues in the context of the "dipole-flip" model, which is known to exhibit nonlinear response. First, we demonstrate how non-Gaussian statistics can be predicted from purely equilibrium molecular dynamics (MD) simulations (i.e., without resort to a full nonequilibrium MD as is the current practice). Second, we show that the Gaussian statistics approximation may also be used to identify the physical origins of nonlinear response residing in a small number of coordinates. Third, we explore an approach for correcting the Gaussian statistics approximation for nonlinear response effects using the same equilibrium simulation. The results are discussed in the context of several other examples of nonlinear responses throughout the literature.

Tests for, origins of, and corrections to non-Gaussian statistics. The dipole-flip model