Probing complex stacking in a layered material via electron-nuclear quadrupolar coupling
arXiv:2212.08895 · doi:10.1103/PhysRevMaterials.7.L091001
Abstract
For layered materials, the interlayer stacking is a critical degree of freedom tuning electronic properties, while its microscopic characterization faces great challenges. The transition-metal dichalcogenide 1T-TaS represents a novel example, in which the stacking pattern is not only enriched by the spontaneous occurrence of the intralayer charge density wave, but also recognized as a key to understand the nature of the low-temperature insulating phase. We exploit the nuclei in a 1T-TaS single crystal as sensitive probes of the local stacking pattern via quadrupolar coupling to the electron density distribution nearby, by combining nuclear magnetic resonance (NMR) measurements with the state-of-the-art first-principles electric-field gradient calculations. The applicability of our proposal is analyzed through temperature, magnetic-field, and angle dependent NMR spectra. Systematic simulations of a single 1T-TaS layer, bilayers with different stacking patterns, and typical stacking orders in three-dimensional (3D) structures unravel distinct NMR characteristics. Particularly, one 3D structure achieves a quantitative agreement with the experimental spectrum, which clearly rationalizes the coexistence of two types of interfacial environments. Our method may find general applications in the studies of layered materials.
References in corpus (20)
- Signatures of moiré-trapped valley excitons in MoSe/WSe heterobilayers
- Magic continuum in twisted bilayer WSe2
- Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides
- Is 1T-TaS a 40 year old quantum spin liquid?
- Orbital textures and charge density waves in transition metal dichalcogenides
- Band insulator to Mott insulator transition in 1T-TaS
- A new high-temperature quantum spin liquid with polaron spins
- Three Dimensional Metallic and Two Dimensional Insulating Behavior in Tantalum Dichalcogenides
- Mottness versus unit-cell doubling as the driver of the insulating state in 1T-TaS2
- Disrupted orbital order and the pseudo-gap in layered 1T-TaS
- Ultrafast doublon dynamics in photo-excited 1T-TaS
- Spinon Fermi surface in a cluster Mott insulator model on a triangular lattice and possible application to 1T-TaS
- Orbital-driven Mottness collapse in 1T-TaS2-xSex transition metal dichalcogenide
- Coexisting localized and itinerant gapless excitations in a quantum spin liquid candidate 1T-TaS
- Distinguishing a Mott Insulator from a Trivial Insulator with Atomic Adsorbates
- Emergent Novel Metallic State in a Disordered 2D Mott Insulator
- Effect of Stacking Order on the Electronic State of 1T-TaS
- Doublon-like excitations and their phononic coupling in a Mott charge-density-wave system
- Understanding the flat band in 1T-TaS2 using a rotated basis
- Renormalization of the Mott gap by lattice entropy: The case of 1T-TaS2