The alloying of first-principles calculations with quasiparticle methodologies for the converged solution of the quantum many-electron states in the correlated compound Iron monoxide

TL;DR

This paper benchmarks various first-principles methods, including hybrid functionals and quasiparticle approaches, to accurately model the correlated electronic states of Iron monoxide, emphasizing the importance of initial wavefunctions and convergence.

Contribution

It systematically compares first-principles methods for Iron monoxide, establishing hybrid functionals as optimal for balancing accuracy and computational efficiency.

Findings

Hybrid functionals provide the best accuracy-efficiency trade-off.

Rigorous convergence of Dyson equations improves electronic state predictions.

Initial wavefunction choice significantly affects convergence and results.

Abstract

Transition metal oxides belong to a genre of quantum materials essential for the exploration of theoretical methods for quantifying electronic correlation. Finding an efficient and accurate first principles method for the assertion of such physical properties is momentous for the predictive modelling of physics based thermoelectric and photovoltaic devices. Prior investigations have suggested that incorporation of the so called random phase approximation for the electronic screening interaction by adding up the electron hole pairs leads to significant improvement in the accuracy of first principle calculations. Nonetheless the method has seldom been adapted systematically for studying the properties of prototypical transition metal oxides, particularly that of the correlated compound Iron monoxide. In this work, we provide a benchmarking study of a variety of first principles methods such as the density functional theory artificially stabilized by Coulomb interactions, Hybrid functionals as well as the quasiparticle Greens function approach to self-energy interactions. A rigorous convergence of the self-consistent Dysons equations have been provided addressing the importance of initial choice of wavefunctions guided by first principles on the converged solutions and the interplay of various orbital degrees of freedom adjacent to the Fermi level. It is momentous to obtain accurate wavefunctions and many-electronic energy states for the quantification of correlation and efficient modelling of oxide interfaces for quantum applications. The study establishes the hybrid functional scheme as the optimal approach for the ideal trade-off between accuracy of the ground state wavefunctions and computational efficiency for large-scale simulations towards the efficient convergence of correlated electronic wavefunctions and low energy electronic properties.