Exploring Coupled Cluster Green's function as a method for treating system and environment in Green's function embedding methods

Abstract

Within the self-energy embedding theory (SEET) framework, we study coupled cluster Green's function (GFCC) method in two different contexts: as a method to treat either the system or environment present in the embedding construction. Our study reveals that when GFCC is used to treat the environment we do not see improvement in total energies in comparison to the coupled cluster method itself. To rationalize this puzzling result, we analyze the performance of GFCC as an impurity solver with a series of transition metal oxides. These studies shed light on strength and weaknesses of such a solver and demonstrate that such a solver gives very accurate results when the size of the impurity is small. We investigate if it is possible to achieve a systematic accuracy of the embedding solution when we increase the size of the impurity problem. We found that in such a case, the performance of the solver worsens, both in terms of finding the ground state solution of the impurity problem as well as the self-energies produced. We concluded that increasing the rank of GFCC solver is necessary to be able to enlarge impurity problems and achieve a reliable accuracy. We also have shown that natural orbitals from weakly correlated perturbative methods are better suited than symmetrized atomic orbitals (SAO) when the total energy of the system is the target quantity.

References in corpus (48)

• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• The GW method
• Quasiparticle Self-Consistent GW Theory
• Resolution-of-identity approach to Hartree-Fock, hybrid density functionals, RPA, MP2, and \textit{GW} with numeric atom-centered orbital basis functions
• First-principles Calculations of the Electronic Structure and Spectra of Strongly Correlated Systems: Dynamical Mean-field Theory
• First principles approach to the electronic structure of strongly correlated systems: combining GW and DMFT
• Measuring orbital interaction using quantum information theory
• Towards the solution of the many-electron problem in real materials: equation of state of the hydrogen chain with state-of-the-art many-body methods
• Extended Dynamical Mean Field Theory and GW method
• Entanglement Measures for Single- and Multi-Reference Correlation Effects
• Compressing Green's function using intermediate representation between imaginary-time and real-frequency domains
• Benchmark of GW approaches for the GW100 testset
• Fully self-consistent GW calculations for atoms and molecules
• Dynamical mean-field theory from a quantum chemical perspective
• Truncated Configuration Interaction expansions as solvers for correlated quantum impurity models and dynamical mean field theory
• Fully self-consistent $GW$ and quasi-particle self-consistent $GW$ for molecules
• The description of strong correlation within self-consistent Green's function second-order perturbation theory
• Sparse sampling approach to efficient ab initio calculations at finite temperature
• When strong correlations become weak: Consistent merging of $GW$ and DMFT
• autoCAS: a program for fully automated multi-configurational calculations
• Gaussian and plane-wave mixed density fitting for periodic systems
• Temperature and bath size in exact diagonalization dynamical mean field theory
• Towards ab initio self-energy embedding theory in quantum chemistry
• Systematically improvable multi-scale solver for correlated electron systems
• Multitier self-consistent $GW$+EDMFT
• Second-order Green's function perturbation theory for periodic systems
• Direct comparison of many-body methods for realistic electronic Hamiltonians
• Finite temperature quantum embedding theories for correlated systems
• Dynamical Mean-Field Theory for Quantum Chemistry
• Self-energy embedding theory (SEET) for periodic systems
• Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory
• Ab Initio Full Cell GW+DMFT for Correlated Materials
• Generalized self-energy embedding theory
• Coupled-cluster impurity solvers for dynamical mean-field theory
• Rigorous ab initio quantum embedding for quantum chemistry using Green's function theory: screened interaction, non-local self-energy relaxation, orbital basis, and chemical accuracy
• Ab-Initio self-energy embedding for the photoemission spectra of NiO and MnO
• Density Functional plus Dynamical Mean-Field Theory of the Spin-Crossover Molecule Fe(phen)${}_2$(NCS)${}_2$
• Efficient temperature-dependent Green's functions methods for realistic systems: compact grids for orthogonal polynomial transforms
• Exploring connections between statistical mechanics and Green's functions for realistic systems. Temperature dependent electronic entropy and internal energy from a self-consistent second-order Green's function
• Chebyshev polynomial representation of imaginary time response functions
• Correlated Electron Pseudopotentials for 3d-Transition Metals
• Fractional charge and spin errors in self-consistent Green's function theory
• Local Hamiltonians for quantitative Green's function embedding methods
• Testing self-energy embedding theory in combination with GW
• Diatomic molecule as a testbed for combining DMFT with electronic structure methods such as $GW$ and DFT
• Approximate Green's Function Coupled Cluster Method Employing Effective Dimension Reduction
• Testing the GFCCSD impurity solver on real materials within the self-energy embedding theory framework
• Combining Density Functional Theory and Green's Function Theory: Range-Separated, Non-local, Dynamic, and Orbital-Dependent Hybrid Functional

Cited by in corpus (4)

• On the effective reconstruction of expectation values from ab initio quantum embedding
• Non-Dyson Algebraic Diagrammatic Construction Theory for Charged Excitations in Solids
• Constructing `full-frequency' spectra via moment constraints for coupled cluster Green's functions
• Triple excitations in Green's function coupled cluster solver for studies of strongly correlated systems in the framework of self-energy embedding theory