Nuclear Quantum Effects on the Charge-Density Wave Transition in NbX₂ (X = S, Se).

Abstract

Understanding the origin of charge-density wave (CDW) instability is important for manipulating novel collective electronic states. Many layered transition metal dichalcogenides (TMDs) share similarity in the structural and electronic instability, giving rise to diverse CDW phases and superconductivity. It is still puzzling that even isostructural and isoelectronic TMDs show distinct CDW features. For instance, bulk NbSe₂ exhibits CDW order at low temperature, while bulk NbS₂ displays no CDW instability. The CDW transitions in single-layer NbS₂ and NbSe₂ are also different. In the classic limit, we investigate the electron correlation effects on the dimensionality dependence of the CDW ordering. By performing <i>ab initio</i> path integral molecular dynamics simulations and comparative analyses, we further revealed significant nuclear quantum effects in these systems. Specifically, the quantum motion of sulfur anions significantly reduces the CDW transition temperature in both bulk and single-layer NbS₂, resulting in distinct CDW features in the NbS₂ and NbSe₂ systems.