Excitonic and lattice contributions to the charge density wave in 1T−TiSe2 revealed by a phonon bottleneck

H Hedayat,S R Clark,E Carpene,J Van Wezel,S Karbassi,C J Sayers,D Bugini,G Cerullo,S Friedemann,C Dallera,E Da Como,T Batten,D Wolverson

doi:10.1103/physrevresearch.1.023029

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.

Highlights

Charge density waves (CDWs) are an important component in phase diagrams of many correlated electron systems [1,2]
The sample temperature is ideal since it is below TCDW = 202 K, but sufficiently high to allow perturbations to the periodic lattice distortion (PLD) as we show below
As confirmation that the energy shift is a dynamic perturbation of the CDW, and not just heating of the valence band (VB) electron distribution, we show in Figs. 1(e) and 1(f) the VB dynamics at 80 and 300 K, respectively

Summary

Introduction

Charge density waves (CDWs) are an important component in phase diagrams of many correlated electron systems [1,2]. Observed in low-dimensional materials, the signatures of a CDW phase have been reported in two-dimensional transition metal dichalcogenides (TMDs) [3], cuprate superconductors [4], π -conjugated polymers [5], and metal oxides [6]. The central importance of CDW states arises from the relationship between fluctuations in their order parameter and superconductivity, Mott insulating states, and spin density waves [1,7]. In the TMD 1T -TiSe2 superconductivity appears in proximity to CDW incommensurability [8], which can be achieved by pressure [9], copper doping [10], or electrostatic gating [11].

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Results

Conclusion