Charge transfer in T/H heterostructures of transition metal dichalcogenides

TL;DR

This study systematically investigates charge transfer in T/H heterostructures of transition metal dichalcogenides, revealing how interlayer distance and composition influence electronic properties and potential Mott insulating or superconducting states.

Contribution

It provides the first comprehensive ab-initio analysis of charge transfer across all relevant T/H bilayers and bulk structures, clarifying the factors affecting electronic correlations.

Findings

Charge transfer depends strongly on interlayer distance.

Se compounds exhibit smaller charge transfer than S compounds.

Bulk 4H_b structures show more charge transfer than bilayers.

Abstract

The $\sqrt{13}\times\sqrt{13}$ charge density wave state of the T polytype of MX$_2$ (M=Nb,Ta, X=S, Se) is known to host a half-filled flat band, which electronic correlations drive into a Mott insulating state. When T polytypes are coupled to strongly metallic H polytypes, such as in T/H bilayer heterostructures or the bulk 4H$_b$ polytype, charge transfer can destabilize the Mott state, but quantifying its magnitude has been a source of controversy. In this work, we perform a systematic ab-initio study of charge transfer for all experimentally relevant T/H bilayers and bulk 4H$_b$ structures. In all cases we find charge transfer from T to H layers which depends strongly on the interlayer distance but weakly on the Hubbard interaction. Additionally, Se compounds display smaller charge transfer than S compounds, and 4H$_b$ bulk polytypes display more charge transfer than isolated bilayers. We rationalize these findings in terms of band structure properties, and argue they might explain differences between compounds observed experimentally. Our work reveals the tendency to Mott insulation and the origin of superconductivity may vary significantly across the family of T/H heterostructures.