Compact sum-over-states expression without dipolar terms for calculating nonlinear susceptibilities

Abstract

Using sum rules, the dipolar terms can be eliminated from the commonly-used sum-over-states (SOS) expression for nonlinear susceptibilities. This new dipole-free expression is more compact, converges to the same results as the common SOS equation, and is more appropriate for analyzing certain systems such as octupolar molecules. The dipole-free theory can be used as a tool for analyzing the uncertainties in quantum calculations of susceptibilities, can be applied to a broader set of quantum systems in the three-level model where the standard SOS expression fails, and more naturally leads to fundamental limits of the nonlinear susceptibilities.