Origin of Distinct Insulating Domains in the Layered Charge Density Wave Material 1T-TaS2

TL;DR

This study combines experimental and theoretical methods to reveal how stacking variations in 1T-TaS2 create distinct insulating domains, including buried Mott insulators that may host quantum spin liquids.

Contribution

It provides new insights into the stacking-dependent electronic structure of 1T-TaS2, identifying buried Mott insulating layers and their role in quantum phenomena.

Findings

Mott-insulating domains transition to band-insulating domains with vertical dimerization

Two distinct band insulating domains are differentiated by band edge broadening

Buried Mott insulating layers are identified, potentially hosting quantum spin liquids

Abstract

Vertical charge order shapes the electronic properties in layered charge density wave (CDW) materials. Various stacking orders inevitably create nanoscale domains with distinct electronic structures inaccessible to bulk probes. Here, the stacking characteristics of bulk 1$T$-TaS$2$ are analyzed using scanning tunneling spectroscopy (STS) and density functional theory (DFT) calculations. It is observed that Mott-insulating domains undergo a transition to band-insulating domains restoring vertical dimerization of the CDWs. Furthermore, STS measurements covering a wide terrace reveal two distinct band insulating domains differentiated by band edge broadening. These DFT calculations reveal that the Mott insulating layers preferably reside on the subsurface, forming broader band edges in the neighboring band insulating layers. Ultimately, buried Mott insulating layers believed to harbor the quantum spin liquid phase are identified. These results resolve persistent issues regarding vertical charge order in 1$T$-TaS$2$, providing a new perspective for investigating emergent quantum phenomena in layered CDW materials.