Chiral charge-density wave in TiSe$_2$ due to photo-induced structural distortions

TL;DR

This paper investigates the origin of the chiral charge-density wave in TiSe$_2$, demonstrating that photo-induced structural distortions lead to non-centrosymmetric structures explaining optical chirality, reconciling previous conflicting theories.

Contribution

It combines experimental pump-probe measurements with first-principles calculations to show photoexcitation induces non-centrosymmetric structures in TiSe$_2$, clarifying the origin of its chiral CDW.

Findings

Photoexcitation causes non-centrosymmetric structures in TiSe$_2$.

Finite optical chirality arises from near-degenerate structures.

Structural distortions are crucial for understanding the CDW in TiSe$_2$.

Abstract

A variety of experiments have been carried out to establish the origin of the chiral charge-density wave transition in 1T-TiSe$_2$, which in turn has led to contradictory conclusions on the origin of this transition. Some studies suggest the transition is a phonon-driven structural distortion while other studies suggest it is an excitonic insulator phase transition that is accompanied by a lattice distortion. First, we propose these interpretations can be reconciled if one analyzes the available experimental and theoretical data within a formal definition of what constitutes an excitonic insulator as initially proposed by Keldysh and Kopaev. Next, we present pump-probe measurements of circularly polarized optical transitions and first-principles calculations where we highlight the importance of accounting for structural distortions to explain the finite chirality of optical transitions in the CDW phase. We show that at the elevated electronic temperature that occurs upon photoexcitation, there is a non-centrosymmetric structure that is near-degenerate in energy with the centrosymmetric charge density wave structure, which explains the finite chirality of the optical transitions observed in the CDW phase of TiSe$_2$.