Diatomic molecule as a testbed for combining DMFT with electronic structure methods such as $GW$ and DFT

Abstract

We implemented combination of DMFT and $GW$ in its fully self-consistent way, one shot $GW$ approximation, and quasiparticle self-consistent scheme, and studied how well these combined methods perform on H${}_2$ molecule as compared to more established methods such as LDA+DMFT. We found that most flavors of $GW$+DMFT break down in strongly correlated regime due to causality violation. Among $GW$+DMFT methods, only the self-consistent quasiparticle $GW$+DMFT with static double-counting, and a new method with causal double-counting, correctly recover the atomic limit at large H-atom separation. While some flavors of $GW$+DMFT improve the single-electron spectra as compared to LDA+DMFT, the total energy is best predicted by LDA+DMFT, for which the exact double-counting is known, and is static.

13pages, 9 figures

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• Testing self-energy embedding theory in combination with GW
• Diagrammatic Monte Carlo Method for Impurity Models with General Interactions and Hybridizations
• Exploring Coupled Cluster Green's function as a method for treating system and environment in Green's function embedding methods
• Quasiparticle and fully self-consistent GW methods: an unbiased analysis using Gaussian orbitals
• Non-local Correlation Effects in Fermionic Many-Body Systems: Overcoming the Non-causality Problem
• Causal optimization method for imaginary-time Green's functions in interacting electron systems
• Measuring the ultrafast screening of $U$ in photo-excited charge-transfer insulators with time-resolved X-ray absorption spectroscopy
• Dual-space cluster-diagrammatic approach to nonlocal electronic correlations
• All-electron Quasiparticle Self-consistent GW for Molecules and Periodic Systems within the Numerical Atomic Orbital Framework