Pushing the hyperpolarizability to the limit

Abstract

We use numerical optimization to find a one-dimensional potential energy function that yields the largest hyperpolarizability, which we find is within 30% of the fundamental limit. Our results reveal insights into the character of the potential energy functions and wavefunctions that lead to the largest hyperpolarizability. We suggest that donor-acceptor molecules with a conjugated bridge with many sites of reduced conjugation to impart conjugation modulation may be the best paradigm for making materials with huge hyperpolarizabilities that approach the fundamental limit.