6533b85afe1ef96bd12ba008

RESEARCH PRODUCT

Calculation of frequency-dependent hyperpolarizabilities using general coupled-cluster models.

Darragh P. O’neillMihály KállayJürgen Gauss

subject

Coupled clusterChemistryGeneral Physics and AstronomyLimit (mathematics)Statistical physicsPhysical and Theoretical ChemistryTriplet stateAtomic physicsQuantum chemistry

description

By exploiting the similarities between response theory and analytic derivative theory, we present a scheme for calculating frequency-dependent hyperpolarizabilities at the coupled-cluster level within the framework for analytic third derivatives. This has been implemented for arbitrary levels of coupled-cluster theory up to the full-configuration-interaction limit. An investigation of some small molecules shows that the inclusion of triple excitations is essential for an accurate description of hyperpolarizabilities.

10.1063/1.2770714https://pubmed.ncbi.nlm.nih.gov/17919013