Symmetry breaking transforms strong to normal correlation and false metals to true insulators

TL;DR

This paper demonstrates that allowing symmetry breaking in electronic structure calculations can convert false metallic predictions into true insulating states in transition-metal oxides, reducing the need for strong correlation treatments.

Contribution

It introduces a symmetry-breaking approach in DFT calculations that explains insulating behavior without relying on strong correlation theories.

Findings

Symmetry breaking lowers energy and correctly predicts insulators.

Broken symmetries remove degeneracies, reducing the need for strong correlation.

The approach distinguishes paramagnetic insulators from metals.

Abstract

Material scientists and condensed matter physicists have long been divided on the issue of choosing the conceptual framework for explaining why open-shell transition-metal oxides tend to be insulators, whereas otherwise successful theories such as DFT often predict them to be (false) metals. Strong correlation becomes the recommended medicine. We point out that strong correlation can be mitigated by allowing DFT to lower the energy by breaking structural, magnetic or dipolar symmetries. Such local motifs are observed experimentally by local probes beyond the 'average structure' determined by X-Ray diffraction. Observed broken symmetries can arise from slow fluctuations that persist over the observation time or longer. The surprising fact is that when symmetry breaking motifs are used as input to electronic structure calculations, false metals are converted into real insulators without the recommended medicine of strong correlation. Consistently, DFT calculations that show energy lowering symmetry breaking correct most cases where DFT, even with advanced exchange-correlation functionals, previously missed the correct metal vs insulator designation. Total energy calculations distinguish systems that support energy-lowering symmetry breaking from those that do not. This approach distinguishes between paramagnetic insulating and metallic phases and shows mass enhancement in Mott metals. The reason is that symmetry breaking removes many of the degeneracies that exist in a symmetry-unbroken system, reducing significantly the need for strong correlation. If one chooses to ignore symmetry breaking, the persistent degeneracies often call for strong correlation treatment. Thus, symmetry breaking transforms strong to normal correlation and false metals to true insulators. This view sheds light on the historic controversy between Mott and Slater that still reverberates today.