TRUNCATED SUM RULES AND THEIR USE IN CALCULATING FUNDAMENTAL LIMITS OF NONLINEAR SUSCEPTIBILITIES

Truncated sum rules have been used to calculate the fundamental limits of the nonlinear susceptibilities and the results have been consistent with all measured molecules. However, given that finite-state models appear to result in inconsistencies in the sum rules, it may seem unclear why the method works. In this paper, the assumptions inherent in the truncation process are discussed and arguments based on physical grounds are presented in support of using truncated sum rules in calculating fundamental limits. The clipped harmonic oscillator is used as an illustration of how the validity of truncation can be tested and several limiting cases are discussed as examples of the nuances inherent in the method.