The improvements in computer hardware and in the development of new, accurate exchange-correlation functionals, have enabled the study of molecular properties for molecules of chemical interest. The combined use of theoretical calculations with experimental observations allows for new insight into the properties of molecules and their electron densities, which in turn may be a useful guide when designing molecular materials with specific properties.
In this talk, I will outline our new framework for calculating any kind of molecular property within a self-consistent field formalism (Hartree-Fock and Kohn-Sham density functional theory), including the study of excited-state properties. The approach is formulated in the atomic orbital basis, allowing large molecules to be studied, as well as using both relativistic and nonrelativistic methodologies.
I will give several examples of linear and nonlinear molecular properties, with particular emphasis on properties involving the nuclear motion in the molecule. These examples will include both properties related to vibrational spectroscopy, with an emphasis on Raman spectroscopies, pure vibrational contributions to nonlinear optical properties and vibronic effects to nonlinear properties.