Ultrafast Stiffening of the Lattice Potential and Metastable State Formation in 1$T$-TiSe$_2$

TL;DR

This study uses ultrafast optical spectroscopy to explore how photoexcitation affects the lattice and electronic states in 1T-TiSe2, revealing ultrafast lattice stiffening and a metastable metallic phase.

Contribution

It uncovers the ultrafast hardening of the CDW amplitude mode as a signature of lattice potential restoration and identifies a critical fluence for metastable state formation.

Findings

CDW amplitude mode exhibits anomalous hardening with increased pump fluence.

A sharp increase in buildup time marks the transition to a metastable metallic state.

Ultrafast restoration of the bare lattice potential is observed.

Abstract

We use ultrafast optical spectroscopy to investigate the electronic and lattice dynamics of the charge-density wave (CDW) material 1$T$-TiSe$_2$ across various temperatures and pump fluences. We reveal a close relationship between the observed ultrafast dynamical processes and two characteristic temperatures: $T_{\rm CDW}$ ($\sim$202 K) and $T^*$ ($\sim$165 K). Two coherent phonon modes are identified: a high-frequency $A_{1g}$ mode ($\omega_{1}$) and a lower-frequency $A_{1g}$ CDW amplitude mode ($\omega_{2}$). In stark contrast to thermal melting, where phonons soften, the CDW amplitude mode exhibits anomalous hardening (frequency upshift) with increasing pump fluence. We establish this hardening as the direct signature of an ultrafast restoration of the bare lattice potential. The photoexcited carrier plasma screens the long-range electron-phonon interactions that drive the Peierls-like instability, effectively ``undressing" the soft phonon and driving its frequency toward the stiffer value of the unrenormalized lattice. Furthermore, an abrupt increase in the excited state buildup time above a critical pump fluence marks a sharp boundary to a photoinduced metastable metallic state. These findings demonstrate that the CDW order in 1$T$-TiSe$_2$ is governed by a fragile, fluence-tunable competition between excitonic correlations and lattice dynamics.