The vector (observable) part of the hyperpolarizability tensor for frequency doubling, βvec( -2ω; ω, ω), is calculated using perturbation theory and the PPP model Hamiltonian. Calculations for a dozen representative molecules show that this method yields results in excellent agreement with experiment both for fairly strong and for quite weak optical non-linearity. Thus PPP-type calculations should be useful in understanding π electron molecular non-linear optical properties.
ASJC Scopus subject areas
- Physical and Theoretical Chemistry
- Condensed Matter Physics
- Atomic and Molecular Physics, and Optics
- Surfaces and Interfaces