Nonlinear response theory—I

Abstract

A general nonlinear response theory for the case of linear coupling of physical systems to arbitrary external fields is formulated for applications in different branches of physics. This is done within the framework of non-relativistic density matrix approach of quantum mechanics. Some simple properties of response functions and other related functions, which are introduced here for convenience, are studied to obtain suitable representations of the nonlinear response functions, including important sum-rules. As an example, the sum rule for the second-order response function is applied to electronic dipole nonlinearity at optical frequencies which includes both the Raman nonlinearity arising from perturbation to the electronic motion from external ionic displacement field and the usual optical sum, difference and harmonic generations. This immediately allows us to visualize a rigorous connection between these two types of non-linearities.