  Nonlinear response occurs naturally when a strong perturbation takes a system
far from equilibrium. Despite of 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
multi-time correlation functions among both time reversal symmetric and
asymmetric observables, which can be evaluated from derivatives of large
deviation functions. This connection establishes a thermodynamic-like 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.
