Ab Initio Many Body Quantum Embedding and Local Correlation in Crystalline Materials using Interpolative Separable Density Fitting

Abstract

We present an efficient implementation of ab initio many-body quantum embedding and local correlation methods for infinite periodic systems through translational symmetry adapted interpolative separable density fitting, an approach which reduces the scaling of the calculations to only linear with the number of k-points. Employing this methodology, we compute correlated ground-state coupled cluster energies within density matrix embedding and local natural orbital correlation frameworks for both weakly and strongly correlated solids, using up to 1000 k-points. By extrapolating the local correlation domains and k-point sampling we further obtain estimates of the full coupled cluster with singles, doubles, and perturbative triples ground-state energies in the thermodynamic limit.

13 pages, 4 figures, and 4 tables

References in corpus (35)

• Recent developments in the PySCF program package
• Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
• Resolution-of-identity approach to Hartree-Fock, hybrid density functionals, RPA, MP2, and \textit{GW} with numeric atom-centered orbital basis functions
• Density matrix embedding: A strong-coupling quantum embedding theory
• Quantum embedding theories
• A practical guide to density matrix embedding theory in quantum chemistry
• Ideal regularization of the Coulomb singularity in exact exchange by Wigner-Seitz truncated interactions: towards chemical accuracy in non-trivial systems
• Efficient Implementation of Ab Initio Quantum Embedding in Periodic Systems: Density Matrix Embedding Theory
• Dynamical mean-field theory from a quantum chemical perspective
• Coupled cluster theory in materials science
• Influence of apical oxygen on the extent of in-plane exchange interaction in cuprate superconductors
• Applying the Coupled-Cluster Ansatz to Solids and Surfaces in the Thermodynamic Limit
• Gaussian and plane-wave mixed density fitting for periodic systems
• Cubic-scaling all-electron GW calculations with a separable density-fitting space-time approach
• Systematically Improvable Tensor Hypercontraction: Interpolative Separable Density-Fitting for Molecules Applied to Exact Exchange, Second- and Third-Order Møller-Plesset Perturbation Theory
• Systematic electronic structure in the cuprate parent state from quantum many-body simulations
• Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory
• Separable Resolution-of-the-Identity with All-Electron Gaussian Bases: Application to Cubic-scaling RPA
• Overcoming the Memory Bottleneck in Auxiliary Field Quantum Monte Carlo Simulations with Interpolative Separable Density Fitting
• Systematic improvability in quantum embedding for real materials
• Cubic scaling algorithms for RPA correlation using interpolative separable density fitting
• Ground-state phase diagram of the three-band Hubbard model from density matrix embedding theory
• Periodic Local Coupled-Cluster Theory for Insulators and Metals
• Interpolative separable density fitting decomposition for accelerating Hartree-Fock exchange calculations within numerical atomic orbitals
• Hamiltonian symmetries in auxiliary-field quantum Monte Carlo calculations for electronic structure
• Low-Scaling Algorithm for the Random Phase Approximation using Tensor Hypercontraction with k-point Sampling
• Downfolding from Ab Initio to Interacting Model Hamiltonians: Comprehensive Analysis and Benchmarking of the DFT+cRPA Approach
• Rigorous screened interactions for realistic correlated electron systems
• On the effective reconstruction of expectation values from ab initio quantum embedding
• Ab initio quantum many-body description of superconducting trends in the cuprates
• Even Faster Exact Exchange for Solids via Tensor Hypercontraction
• A Critical Analysis of Least-Squares Tensor Hypercontraction Applied to MP3
• Optimization strategies developed on NiO for Heisenberg exchange coupling calculations using projector augmented wave based first-principles DFT+U+J
• A static quantum embedding scheme based on coupled cluster theory
• Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2