Interacting-Bath Dynamical Embedding for Capturing Nonlocal Electron Correlation in Solids
Jiachen Li, Tianyu Zhu
Abstract
Quantitative simulation of electronic structure of solids requires treating local and nonlocal electron correlations on an equal footing. We present a new ab initio formulation of Green's function embedding which, unlike dynamical mean-field theory that uses noninteracting bath, derives bath representation with general two-particle interactions in a systematically improvable manner. The resulting interacting-bath dynamical embedding theory (ibDET) utilizes an efficient real-axis coupled-cluster solver to compute the self-energy, approaching the full system limit at much reduced cost. When combined with the GW theory, GW+ibDET achieves good agreement with experimental spectral properties across a range of semiconducting, insulating, and metallic materials. Our approach also enables quantifying the role of nonlocal electron correlation in determining material properties and addressing the long-standing debate on the bandwidth narrowing of metallic sodium.