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Nonlinear transport coefficients from large deviation functions.

Nonlinear response occurs naturally when a strong perturbation takes a system far from equilibrium. Despite its omnipresence in nanoscale systems, it is difficult to predict in a general and efficient way. Here, we introduce a way to compute arbitrarily high order transport coefficients of stochastic systems, using the framework of large deviation theory. Leveraging time reversibility in the microscopic dynamics, we relate nonlinear response to equilibrium multitime correlation functions among both time reversal symmetric and asymmetric observables, which can be evaluated from derivatives of large deviation functions. This connection establishes a thermodynamiclike relation for nonequilibrium response and provides a practical route to its evaluation, as large deviation functions are amenable to importance sampling. We demonstrate the generality and efficiency of this method in predicting transport coefficients in single particle systems and an interacting system exhibiting thermal rectification.