Simulating one hundred entangled atoms using projected-interacting full configuration interaction wavefunctions corrected by projected density functionals

Abstract

Simulating entangled atoms is a prerequisite to modeling quantum materials and remains an outstanding challenge for theory. I introduce a correlated wavefunction approach capable of simulating large entangled systems, and demonstrate its application to a 300-electron active space. Projected-interacting full configuration interaction plus density functional theory PiFCI+DFT combines near-exact correlated wavefunctions of multiple partially-interacting model systems, each corrected by a formally exact density functional. This approach can access large active spaces and visualize entanglement and strong correlation while maintaining competitive accuracy for molecular properties.