Dalgarno-Lewis perturbation theory for nonlinear optics

TL;DR

This paper introduces a quadrature-based Dalgarno-Lewis perturbation method for calculating nonlinear optical responses in quantum systems, enabling exact polarizability expressions from ground state wave functions without explicit potential dependence.

Contribution

The paper extends the Dalgarno-Lewis perturbation theory to nonlinear optics and time-harmonic perturbations, providing a new approach that simplifies calculations and avoids excited state complexities.

Findings

Derived exact expressions for first three electronic polarizabilities.

Extended Dalgarno-Lewis method to time-harmonic perturbations.

Demonstrated method's sensitivity to variational and numerical solutions.

Abstract

We apply the quadrature-based perturbation method of Dalgarno and Lewis to the evaluation of the nonlinear optical response of quantum systems. This general operator method for perturbation theory allows us to derive exact expressions for the first three electronic polarizabilities which require only a good estimate of the ground state wave function, makes no explicit reference to the underlying potential, and avoids complexities arising from excited state degeneracies. We apply this method to simple examples in 1D quantum mechanics for illustration, exploring the sensitivity of this method to variational solutions as well as poor numerical sampling. Finally, to the best of our knowledge, we extend the Dalgarno-Lewis method for for the first time to time-harmonic perturbations, allowing dispersion characteristics to be determined from the unperturbed ground state wave function alone.