Potential energy optimization and Monte Carlo simulations of the first hyperpolarizability: a comparative study

摘要

We contrast two numerical approaches that are used to optimize the intrinsic hyperpolarizability: potential optimization and sum-rule-constrained Monte Carlo simulations. Our aim is to resolve inconsistencies between the two. We show that while the first method accurately reflects the properties of real physical systems, the second requires exotic hamiltonians that obey sum rules but may not represent a physical reality. Under certain extreme conditions, the sum-rule-constrained approach leads to systems that may not be representable by any Schrodinger Equation in differential equation form.© (2012) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.