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Abstract

The 13x 13 charge density wave state of the T polytype of MX2 (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 4Hb 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 4Hb 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 4Hb 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.