Phonon collapse and van der Waals melting of the 3D charge density wave of VSe$_2$

TL;DR

This study reveals that the 3D charge density wave in VSe₂ is driven by acoustic phonon mode collapse and is influenced by electron-phonon interactions and van der Waals forces, providing insights into the mechanisms of CDW formation and melting.

Contribution

It demonstrates the role of phonon softening, electron-phonon coupling, and van der Waals interactions in the formation and melting of 3D CDWs in VSe₂, supported by experimental and first-principles calculations.

Findings

Collapse of an acoustic phonon mode drives the CDW transition.

Electron-phonon interaction peaks at the CDW wavevector.

Van der Waals interactions are essential for CDW melting.

Abstract

Among transition metal dichalcogenides (TMDs), VSe$_2$ is considered to develop a purely 3-dimensional (3D) charge-density wave (CDW) at T$_{CDW}$=110 K. Here, by means of high resolution inelastic x-ray scattering (IXS), we show that the CDW transition is driven by the collapse of an acoustic mode at the critical wavevector \textit{q}$_{CDW}$= (2.25 0 0.7) r.l.u. and critical temperature T$_{CDW}$=110 K. The softening of this mode starts to be pronounced for temperatures below 2$\times$ T$_{CDW}$ and expands over a rather wide region of the Brillouin zone, suggesting a large contribution of the electron-phonon interaction to the CDW formation. This interpretation is supported by our first principles calculations that determine a large momentum-dependence of the electron-phonon interaction, peaking at the CDW wavevector, in the presence of nesting. Fully anharmonic {\it ab initio} calculations confirm the softening of one acoustic branch at \textit{q}$_{CDW}$ as responsible for the CDW formation and show that van der Waals interactions are crucial to melt the CDW. Our work also highlights the important role of out-of-plane interactions to describe 3D CDWs in TMDs.