At ambient pressure, bulk 2H-NbS2 displays no charge density wave instability, which is at odds with the isostructural and isoelectronic compounds 2H-NbSe2, 2H-TaS2, and 2H-TaSe2, and in disagreement with harmonic calculations. Contradictory experimental results have been reported in supported single layers, as 1H-NbS2 on Au(111) does not display a charge density wave, whereas 1H-NbS2 on 6H-SiC(0001) endures a 3 × 3 reconstruction. Here, by carrying out quantum anharmonic calculations from first-principles, we evaluate the temperature dependence of phonon spectra in NbS2 bulk and single layer as a function of pressure/strain. For bulk 2H-NbS2, we find excellent agreement with inelastic X-ray spectra and demonstrate the removal of charge ordering due to anharmonicity. In the two-dimensional limit, we find an enhanced tendency toward charge density wave order. Freestanding 1H-NbS2 undergoes a 3 × 3 reconstruction, in agreement with data on 6H-SiC(0001) supported samples. Moreover, as strains smaller than 0.5% in the lattice parameter are enough to completely remove the 3 × 3 superstructure, deposition of 1H-NbS2 on flexible substrates or a small charge transfer via field-effect could lead to devices with dynamical switching on/off of charge order.
Keywords: Transition metal dichalcogenide; anharmoncity; charge density wave; monolayer; phonons; size-dependent properties.