Multiple Softening Q-vectors Driving a Cascade of CDW Phases in $\mathrm{1T-VSe}_{2}$

TL;DR

This study reveals a cascade of phonon-driven structural transformations leading to a common charge density wave ground state in monolayer 1T-VSe2, highlighting the complex pathways of CDW formation.

Contribution

It introduces a unified phonon-driven cascade mechanism explaining hierarchical CDW phases in monolayer 1T-VSe2 through iterative first-principles calculations.

Findings

Multiple transformation pathways converge to the same low-energy CDW phase.

Intermediate structures remain dynamically unstable and undergo symmetry-lowering distortions.

Different phonon-driven routes can lead to nearly degenerate stable phases.

Abstract

Charge density wave (CDW) formation in two-dimensional materials is governed by complex competing lattice instabilities that remain incompletely understood. Here, we investigate the structural evolution of monolayer $\mathrm{1T-VSe}_{2}$ using first-principles electronic and phonon calculations. The pristine phase exhibits several imaginary-frequency phonon modes associated with dominant instability wave vectors $\mathrm{Q}_{CDW}$, which generate the first-generation CDW phases. Subsequent phonon analyses reveal that several of these intermediate structures remain dynamically unstable and undergo further symmetry-lowering distortions into larger superstructures. Through iterative phonon-driven relaxations, we identify multiple transformation pathways that converge toward the same low-energy $2\sqrt{3}\times4$ CDW configuration. Although these pathways originate from distinct intermediate CDW states, they ultimately reach nearly degenerate energetically stable phases, demonstrating that different phonon-driven routes can lead to the same ground-state configuration. The results establish a unified phonon-driven cascade mechanism for hierarchical CDW formation in monolayer $\mathrm{1T-VSe}_{2}$ and provide a systematic framework for understanding competing ordered phases in low-dimensional quantum materials.