Optimizing the Integration of Multireference Electronic Structure Methods with Non-Equilibrium Green's Functions

A quantum revolution is underway bringing with it a new generation of novel nanoscale sensors and electronic devices with non-classical charge transport characteristics. Describing these fundamentally quantum devices requires a fully quantum transport approach that consistently captures both dynamic and multireference electron correlation effects. This remains a major challenge for many transport methodologies due to limitations in their underlying electronic structure methods. We previously introduced a unique methodology [J. Chem. Phys. 155, 114115 (2021)] for integrating multiconfigurational electronic structure methods within a non-equilibrium Green’s function (NEGF) formalism. I will discuss improvements to this methodology and analyze the relative importance of multireference correlation in characterizing non-classical charge transport effects.