Unveiling Charge-Density Wave, Superconductivity, and Their Competitive Nature in Two-Dimensional NbSe₂

Recently, charge-density wave (CDW) and superconductivity are observed to coexist in atomically thin metallic NbSe₂. Lacking of knowledge on the structural details of CDW, however, prevents us to explore its interplay with superconductivity. Using first-principles calculations, we identify the ground state 3 × 3 CDW atomic structure of monolayer NbSe₂, which is characterized by the formation of triangular Nb clusters and shows a scanning tunnelling microscopy (STM) image and Raman CDW modes in good agreement with experiments. We further demonstrate that from bulk to monolayer NbSe₂, as the layer thickness decreases, the CDW order is gradually enhanced with rising energy gain and strengthened Fermi surface gapping, while superconductivity is weakened due to the increasingly reduced Fermi level density of states in the CDW state. These results well explain the observed opposite thickness dependencies of CDW and superconducting transition temperatures and uncover the nature of competitive interaction between the two collective orders in two-dimensional NbSe₂.