Capturing Long-Range Electron Correlation in Ab Initio Green's Function Embedding

We present an ab initio interacting-bath dynamical embedding theory (ibDET) for accurate treatment of local and long-range electron interactions in periodic systems. The dynamical mean-field theory (DMFT) and its cluster extension has achieved success in simulating correlated materials, but it remains a significant challenge to capture long-range electron correlation and preserve transitional symmetry. In this work, instead of fitting fictitious non-interacting bath orbitals from hybridization function, we derive a set of interacting bath orbitals including cluster-specific natural orbitals using a projective approach. The self-energy calculated from the embedding problem can then be rotated back to the full system to capture long-range physics more accurately. Using the coupled-cluster Green's function method as the impurity solver, we apply the GW+ibDET approach to study spectral properties of two-dimensional boron nitride, magnesium oxide, and bulk sodium, and obtain good agreement with experimental measurements.