Hidden Mott insulator in metallic PdCrO$_2$

TL;DR

This study uses advanced theoretical methods to demonstrate that PdCrO$_2$ contains Mott insulating CrO$_2$ layers within a metallic matrix, revealing complex electron interactions and tunable electronic states.

Contribution

It provides the first detailed theoretical confirmation of hidden Mott insulating layers in PdCrO$_2$ and explores how doping can manipulate these states.

Findings

CrO$_2$ layers are Mott insulating despite metallic behavior

Spectral functions match experimental photoemission data

Oxygen vacancies can induce a transition to itinerant electronic states

Abstract

There has been a long-standing debate on the coexistence between itinerant electrons and localized spins in the PdCrO$_2$ delafossite. By means of the charge self-consistent combination of density functional theory and dynamical mean-field theory, it is corroborated that despite overall remarkable metallic response, the CrO$_2$ layers are indeed Mott insulating as suggested by previous experimental work. The resulting ${\bf k}$-resolved spectral function in the paramagnetic phase is in excellent agreement with available photoemission data. Subtle coupling between the itinerant and Mott-localized degrees of freedom is revealed. Different doping scenarios are simulated in order to manipulate the electronic states within the inert layers. In particular, oxygen vacancies prove effective in turning the hidden Mott insulator into a strongly correlated itinerant subsystem. The present results may open a new venue in research on quantum materials beyond canonical classification schemes.