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 $1T\text{−}\mathrm{Ta}{\mathrm{S}}_2$ 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 ${}^{33}\mathrm{S}$ nuclei in a $1T\text{−}\mathrm{Ta}{\mathrm{S}}_2$ 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 $1T\text{−}\mathrm{Ta}{\mathrm{S}}_2$ 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.

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• Electronic structure
• First-principles calculations
• 2-dimensional systems
• Transition metal dichalcogenides
• Density functional calculations
• Density functional theory
• Nuclear magnetic resonance