Axial-Bonding-Driven Dimensionality Effect on the Charge-Density Wave in NbSe 2 .

2 H -NbSe 2 is a prototypical charge-density-wave (CDW) system, exhibiting such a symmetry-breaking quantum ground state in its bulk and down to a single-atomic-layer limit. However, how this state depends on dimensionality and what governs the dimensionality effect remain controversial. Here, we experimentally demonstrate a robust 3 × 3 CDW phase in both freestanding and substrate-supported bilayer NbSe 2 , far above the bulk transition temperature. We exclude environmental effects and reveal a strong temperature and thickness dependence of Raman intensity from an axially vibrating A 1g phonon mode, involving Se ions. Using first-principles calculations, we show that these result from a delicate but profound competition between the intra- and interlayer bonding formed between Se-p z orbitals. Our results suggest the crucial role of Se out-of-plane displacement in driving the CDW distortion, revealing the Se-dominated dimensionality effect and establishing a new perspective on the chemical bonding and mechanical stability in layered CDW materials.