Recursive calculation of high-order molecular response properties

Abstract

This thesis presents the implementation and application of a computer program for the open-ended calculation of response properties of molecular systems. Using recursive programming techniques, a recently published formulation of response theory can be implemented in a manner that allows the calculation of response properties to arbitrary order. The limitations of the code are dictated by the limitations of connected modules that provide perturbed one- and two-electron integral contributions and exchange and correlation contributions. The properties available from the code are used for a selection of applications: The calculation of the cubic force constants of the second hyperpolarizability of HSOH at the Hartree-Fock level, cubic and quartic force constants of various organic molecules at the density-functional theory (DFT) level, pure vibrational contributions to the polarizability and first hyperpolarizability of retinal and retinal derivatives at the DFT level, and hyper-Raman spectra of two conformations of retinal at the DFT level.