A general time-domain formulation of equation-of-motion coupled-cluster theory for linear spectroscopy

Abstract

A time-dependent (TD) formulation of equation-of-motion (EOM) coupled-cluster (CC) theory is developed, which, unlike other similar TD-EOM-CC approaches [D. R. Nascimento and A. E. DePrince III, J. Chem. Theory Comput. 12, 5834-5840 (2016)], can be applied to any type of linear electronic spectroscopy. The TD-EOM-CC method is formally equivalent to the standard frequency-domain formulation of EOM-CC theory, with a potential computational advantage of a comparatively low memory footprint. This general TD-EOM-CC framework is applied to the linear absorption and electric circular dichroism spectra of several small oxirane derivatives.