Systematic improvability in quantum embedding for real materials

Abstract

Quantum embedding methods have become a powerful tool to overcome deficiencies of traditional quantum modelling in materials science. However, while these are systematically improvable in principle, in practice it is rarely possible to achieve rigorous convergence and often necessary to employ empirical parameters. Here, we formulate a quantum embedding theory, building on the methods of density-matrix embedding theory combined with local correlation approaches from quantum chemistry, to ensure the ability to systematically converge properties of real materials with accurate correlated wave~function methods, controlled by a single, rapidly convergent parameter. By expanding supercell size, basis set, and the resolution of the fluctuation space of an embedded fragment, we show that the systematic improvability of the approach yields accurate structural and electronic properties of realistic solids without empirical parameters, even across changes in geometry. Results are presented in insulating, semi-metallic, and more strongly correlated regimes, finding state of the art agreement to experimental data.

References in corpus (14)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Quantum embedding theories
• Double Counting in LDA+DMFT - The Example of NiO
• Coupled cluster theory in materials science
• Applying the Coupled-Cluster Ansatz to Solids and Surfaces in the Thermodynamic Limit
• Gaussian and plane-wave mixed density fitting for periodic systems
• Spectral Properties of Correlated Materials: Local Vertex and Non-Local Two-Particle Correlations from Combined GW and Dynamical Mean Field Theory
• Electronic structure induced reconstruction and magnetic ordering at the LaAlO${}_3|$SrTiO${}_3$ interface
• Local embedding of Coupled Cluster theory into the Random Phase Approximation using plane-waves
• Rotationally invariant slave-boson and density matrix embedding theory: A unified framework and a comparative study on the 1D and 2D Hubbard Model
• Energy-weighted density matrix embedding of open correlated chemical fragments
• Fully Algebraic and Self-consistent Effective Dynamics in a Static Quantum Embedding
• Extending Density Matrix Embedding: A Static Two-Particle Theory

Cited by in corpus (23)

• Towards near-term quantum simulation of materials
• Surface science using coupled cluster theory via local Wannier functions and in-RPA-embedding: the case of water on graphitic carbon nitride
• Periodic Local Coupled-Cluster Theory for Insulators and Metals
• On the effective reconstruction of expectation values from ab initio quantum embedding
• Rigorous screened interactions for realistic correlated electron systems
• Extending Density Matrix Embedding: A Static Two-Particle Theory
• Bootstrap Embedding on a Quantum Computer
• Fault-tolerant quantum algorithms for quantum molecular systems: A survey
• Multiscale Embedding for Quantum Computing
• Advances in Quantum Defect Embedding Theory
• A static quantum embedding scheme based on coupled cluster theory
• Interacting-bath dynamical embedding for capturing non-local electron correlation in solids
• Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2
• ByteQC: GPU-Accelerated Quantum Chemistry Package for Large-Scale Systems
• Ground-States for Metals from Converged Coupled Cluster Calculations
• Next-generation EDIpack: A Lanczos-based package for quantum impurity models featuring general broken-symmetry phases, flexible bath topologies and multi-platform interoperability
• Unitary transformations within density matrix embedding approaches: A novel perspective on the self-consistent scheme for electronic structure calculation
• Local Potential Functional Embedding Theory of Molecular Systems: Localized Orbital-Based Embedding from an Exact Density-Functional Perspective
• On the pure state $v$-representability of density matrix embedding theory
• Ab Initio Many Body Quantum Embedding and Local Correlation in Crystalline Materials using Interpolative Separable Density Fitting
• Orbital Expansion Variational Quantum Eigensolver: Enabling Efficient Simulation of Molecules with Shallow Quantum Circuit
• Resolving Finite-Size Errors in EOM-CCSD Band Gaps of Solids with Interacting-Bath Dynamical Embedding Theory
• Quantitative Description of Strongly Correlated Materials by Combining Downfolding Techniques and Tensor Networks