On the crystal field in the modern solid-state theory

TL;DR

This paper advocates for an extended crystal-field approach incorporating spin-orbit coupling and electron correlations, presenting the Quantum Atomistic Solid-State Theory (QUASST) to unify descriptions of magnetic and electronic properties in complex materials.

Contribution

It introduces QUASST, an advanced crystal-field theory that accounts for strong correlations and inter-site interactions, unifying 3d and rare-earth compounds in a comprehensive framework.

Findings

Correlated macroscopic properties with atomic-scale electronic structure.

Unified description of 3d and 4f/5f compounds.

Supports unquenching orbital magnetism in 3d oxides.

Abstract

We point out the high physical correctness of the use and the concept of the crystal-field approach, even if is used to metallic magnetic materials of transition-metal 3d/4f/5f compounds. We discuss the place of the crystal-field theory in modern solid-state physics and we point out the necessity to consider the crystal-field approach with the spin-orbit coupling and strong electron correlations, as a contrast to the single-electron version of the crystal field customarily used for 3d electrons. We have extended the strongly-correlated crystal-field theory to a Quantum Atomistic Solid-State Theory (QUASST) to account for the translational symmetry and inter-site spin-dependent interactions indispensable for formation of magnetically-ordered state. We have correlated macroscopic magnetic and electronic properties with the atomic-scale electronic structure for ErNi5, UPd2Al3, FeBr2, LaCoO3 and LaMnO3. In QUASST we have made unification of 3d and rare-earth compounds in description of the low-energy electronic structures and magnetism of open 3d-/4f-/5f-shell electrons. QUASST offers consistent description of zero-temperature properties and thermodynamic properties of 4f-/5f-/3d-atom containing compounds. Our studies indicate that it is the highest time to unquench the orbital magnetism in 3d oxides.