Quantum Embedding Theory for Strongly-correlated States in Materials

Abstract

Quantum embedding theories are promising approaches to investigate strongly-correlated electronic states of active regions of large-scale molecular or condensed systems. Notable examples are spin defects in semiconductors and insulators. We present a detailed derivation of a quantum embedding theory recently introduced, which is based on the definition of effective Hamiltonians. The effect of the environment on a chosen active space is accounted for through screened Coulomb interactions evaluated using density functional theory. Importantly, the random phase approximation is not required and the evaluation of virtual electronic orbitals is circumvented with algorithms previously developed in the context of calculations based on many-body perturbation theory. In addition, we generalize the quantum embedding theory to active spaces composed of orbitals that are not eigenstates of Kohn-Sham Hamiltonians. Finally, we report results for spin defects in semiconductors.

References in corpus (48)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Wannier90: A Tool for Obtaining Maximally-Localised Wannier Functions
• Maximally localized Wannier functions: Theory and applications
• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• Electron-phonon interactions from first principles
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• Quantum computing with defects
• Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
• Density matrix embedding: A simple alternative to dynamical mean-field theory
• Strength of effective Coulomb interactions in graphene and graphite
• Calculations of Hubbard U from first-principles
• Properties of nitrogen-vacancy centers in diamond: group theoretic approach
• Self-consistent hybrid functional for condensed systems
• Hubbard parameters from density-functional perturbation theory
• Low-energy spectrum of iron-sulfur clusters directly from many-particle quantum mechanics
• Hubbard U and Hund's Exchange J in Transition Metal Oxides: Screening vs. Localization Trends from Constrained Random Phase Approximation
• Quantum embedding theories
• A practical guide to density matrix embedding theory in quantum chemistry
• Electrical and optical control of single spins integrated in scalable semiconductor devices
• The negatively charged nitrogen-vacancy centre in diamond: the electronic solution
• Ab-initio procedure for effective models of correlated materials with entangled band structure
• New infrared emission of the NV centre in diamond: Zeeman and uniaxial stress studies
• Quantum simulations of materials on near-term quantum computers
• Nonempirical Range-separated Hybrid Functionals for Solids and Molecules
• State-selective intersystem crossing in nitrogen-vacancy centers
• Electronic Structure Calculation by First Principles for Strongly Correlated Electron Systems
• Screening of Coulomb interactions in transition metals
• Environmentally-Sensitive Theory of Electronic and Optical Transitions in Atomically-Thin Semiconductors
• Discovering correlated fermions using quantum Monte Carlo
• Method for calculating the electronic structure of correlated materials from a truly first-principles LDA+U scheme
• Dielectric dependent hybrid functionals for heterogeneous materials
• Designing defect-based qubit candidates in wide-gap binary semiconductors for solid-state quantum technologies
• The effect of double counting, spin density, and Hund interaction in the different DFT+$U$ functionals
• Coupled-cluster impurity solvers for dynamical mean-field theory
• On the limitations of cRPA downfolding
• 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
• A finite field approach to solving the Bethe Salpeter equation
• Electronic structure of the neutral silicon-vacancy center in diamond
• Derivation of Static Low-Energy Effective Models by ab initio Downfolding Method without Double Counting of Coulomb Correlations: Application to SrVO3, FeSe and FeTe
• Periodic Subsystem Density-Functional Theory
• Downfolded Self-Energy of Many-Electron Systems
• First-principles Studies of Strongly Correlated States in Defect Spin Qubits in Diamond
• Dynamical configuration interaction: Quantum embedding that combines wave functions and Green's functions
• Low-energy effective Hamiltonians for correlated electron systems beyond density functional theory
• A Finite-field Approach for $GW$ Calculations Beyond the Random Phase Approximation
• Decomposition and embedding in the stochastic $GW$ self-energy
• Ab-initio Low-Energy Model of Transition-Metal-Oxide Heterostructure LaAlO3/SrTiO3
• $\text{Ab initio}$ derivation of effective Hamiltonian for La${}_2$CuO${}_4$/La${}_{1.55}$Sr${}_{0.45}$CuO${}_4$ heterostructure

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