Geminal-based configuration interaction

Abstract

The antisymmetrized geminal power (AGP) wave function has a long history and considerable conceptual appeal, but in many situations its accuracy is wanting. Here, we consider a form of configuration interaction (CI) based upon the AGP wave function and take advantage of its killing operators to construct an excitation manifold. Our geminal CI reduces to standard single-determinant-based CI in the limit in which AGP reduces to a single determinant. It substantially improves upon AGP in the reduced BCS Hamiltonian, which serves as a prototype for the kinds of strong pairing correlations relevant in Bardeen-Cooper-Schrieffer-style superconductivity. Moreover, our geminal CI naturally generalizes to add correlation to more general geminal-based wave functions than AGP.