Charge order from structured coupling in VSe$_2$

Abstract

Charge order–ubiquitous among correlated materials–is customarily described purely as an instability of the electronic structure. However, the resulting theoretical predictions often do not match high-resolution experimental data. A pertinent case is 1T1T-VSe_22, whose single-band Fermi surface and weak-coupling nature make it qualitatively similar to the Peierls model underlying the traditional approach. Despite this, its Fermi surface is poorly nested, the thermal evolution of its charge density wave (CDW) ordering vectors displays an unexpected jump, and the CDW gap itself evades detection in direct probes of the electronic structure. We demonstrate that the thermal variation of the CDW vectors is naturally reproduced by the electronic susceptibility when incorporating a structured, momentum-dependent electron-phonon coupling, while the evasive CDW gap presents itself as a localized suppression of spectral weight centered above the Fermi level. Our results showcase the general utility of incorporating a structured coupling in the description of charge ordered materials, including those that appear unconventional.