Dynamical Mean Field Theory for Diatomic Molecules and the Exact Double Counting

Abstract

Dynamical mean field theory (DMFT) combined with the local density approximation (LDA) is widely used in solids to predict properties of correlated systems. In this paper, its application to one of the simplest strongly correlated systems, the hydrogen molecule H${}_2$, is demonstrated to develop a parameter-free LDA+DMFT framework. We propose a method to calculate the exact intersection of LDA and DMFT that leads to highly accurate subtraction of the doubly counted correlation in both methods. When the exact double-counting treatment and a good projector to the correlated subspace are used, LDA+DMFT yields very accurate total energy and excitation spectrum of the H${}_2$ molecule. We also discuss how this double-counting scheme can be extended to solid state calculations.

arXiv comment5 pages, 3 figures

References in corpus (17)

• Maximally-localized generalized Wannier functions for composite energy bands
• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
• Quantum Monte Carlo Impurity Solver for Cluster DMFT and Electronic Structure Calculations in Adjustable Base
• Dynamical Mean-Field Theory within the Full-Potential Methods: Electronic structure of Ce-115 materials
• Mott transition and suppression of orbital fluctuations in orthorhombic 3$d^1$ perovskites
• Hybridization expansion impurity solver: General formulation and application to Kondo lattice and two-orbital models
• Full orbital calculation scheme for materials with strongly correlated electrons
• Plane-wave based electronic structure calculations for correlated materials using dynamical mean-field theory and projected local orbitals
• Levels of self-consistency in the GW approximation
• Dynamical mean-field theory from a quantum chemical perspective
• Covalency in transition metal oxides within all-electron Dynamical Mean Field Theory
• Dynamical Mean-Field Theory for Quantum Chemistry
• Dynamical Mean-Field Theory for Molecular Electronics: Electronic Structure and Transport Properties
• Covalency and the metal-insulator transition in titanate and vanadate perovskites
• Dynamical Mean-Field Theory for Molecules and Nanostructures
• Construction of Localized Basis for Dynamical Mean Field Theory

Cited by in corpus (8)

• Exact double-counting in combining the Dynamical Mean Field Theory and the Density Functional Theory
• Towards ab initio self-energy embedding theory in quantum chemistry
• Correlated materials design: prospects and challenges
• Low-energy effective Hamiltonians for correlated electron systems beyond density functional theory
• Realistic theory of electronic correlations in nanoscopic systems
• Diatomic molecule as a testbed for combining DMFT with electronic structure methods such as $GW$ and DFT
• Quantum embedding for molecules using auxiliary particles -- The ghost Gutzwiller Ansatz
• Combining Density Functional Theory and Green's Function Theory: Range-Separated, Non-local, Dynamic, and Orbital-Dependent Hybrid Functional