First-Principles Theory of Momentum Dependent Local Ansatz Approach to Correlated Electron System

TL;DR

This paper extends the momentum-dependent local-ansatz (MLA) wavefunction method to first-principles calculations using LDA+U Hamiltonian, accurately describing correlated electrons in real materials like paramagnetic Fe.

Contribution

It introduces a first-principles MLA approach that captures electron correlations and low-energy excitations in solids, validated on iron with quantitative results.

Findings

Mass enhancement factor in Fe is 1.65, matching experimental data.

Inter-orbital charge-charge correlations significantly affect correlation energy.

Intra- and inter-orbital spin-spin correlations dominate local moment and mass enhancement.

Abstract

We have extended the momentum-dependent local-ansatz (MLA) wavefunction method to the first-principles version using the tight-binding LDA+U Hamiltonian for the description of correlated electrons in the real system. The MLA reduces to the Rayleigh-Schr\"odinger perturbation theory in the weak correlation limit, and describes quantitatively the ground state and related low-energy excitations in solids. The theory has been applied to the paramagnetic Fe. The role of electron correlations on the energy, charge fluctuations, amplitude of local moment, momentum distribution functions, as well as the mass enhancement factor in Fe has been examined as a function of Coulomb interaction strength. It is shown that the inter-orbital charge-charge correlations between $d$ electrons make a significant contribution to the correlation energy and charge fluctuations, while the intra-orbital and inter-orbital spin-spin correlations make a dominant contribution to the amplitude of local moment and the mass enhancement in Fe. Calculated partial mass enhancements are found to be 1.01, 1.01, and 3.33 for $s$, $p$, and $d$ electrons, respectively. The averaged mass enhancement 1.65 is shown to be consistent with the experimental data as well as the recent results of theoretical calculations.