Excitonic and lattice contributions to the charge density wave in 1T-TiSe$_2$ revealed by a phonon bottleneck

TL;DR

This study uses ultrafast spectroscopy to disentangle excitonic and phononic effects in the charge density wave transition of 1T-TiSe2, revealing a phonon bottleneck and the interplay of these interactions.

Contribution

It demonstrates the combined use of TR-ARPES and TRR to identify the roles of excitonic and phononic interactions in the CDW phase transition of 1T-TiSe2, highlighting a phonon bottleneck phenomenon.

Findings

Identification of a phonon bottleneck at high fluence

Correlation between valence band shift and CDW gap closure

Role of excitonic and phononic interactions in CDW transition

Abstract

Understanding collective electronic states such as superconductivity and charge density waves is pivotal for fundamental science and applications. The layered transition metal dichalcogenide 1T-TiSe2 hosts a unique charge density wave (CDW) phase transition whose origins are still not fully understood. Here, we present ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) measurements complemented by time-resolved reflectivity (TRR) which allows us to establish the contribution of excitonic and electron-phonon interactions to the CDW. We monitor the energy shift of the valence band (VB) and coupling to coherent phonons as a function of laser fluence. The VB shift, directly related to the CDW gap closure, exhibits a markedly slower recovery dynamics at fluences above Fth = 60 microJ cm-2. This observation coincides with a shift in the relative weight of coherently coupled phonons to higher frequency modes in time-resolved reflectivity (TRR), suggesting a phonon bottleneck. Using a rate equation model, the emergence of a high-fluence bottleneck is attributed to an abrupt reduction in coupled phonon damping and an increase in exciton dissociation rate linked to the loss of CDW superlattice phonons. Thus, our work establishes the important role of both excitonic and phononic interactions in the CDW phase transition and the advantage of combining complementary femtosecond techniques to understand the complex interactions in quantum materials.