Transient three-dimensional structural dynamics in 1T−TaSe2

Abstract

We report on thermal and optically driven transitions between the commensurate (C) and incommensurate (IC) charge-density wave (CDW) phases of 1T-TaSe 2. Optical excitation results in suppression of the C-CDW on a subpicosecond timescale. The optically driven C to IC transition involves a short-lived (∼1 ps) unreconstructed phase. Nucleation of an IC phase stacking order is observed already at ∼4 ps following photoexcitation. The short timescales involved in establishing the stacking order implies that the nucleation of the IC phase is influenced by the local geometry of the adjacent layers such that the stacking direction of the C phase determines the stacking direction of the IC phase. From this follows that the nucleation of the IC-CDW is inherently three dimensional (3D). We observe the activation of a coherent shear mode in the optically driven transitions to the transiently stabilized unreconstructed phase. The activation mechanism starts with a rapid lifting of the periodic lattice distortions (PLD) of the Ta sublattice which results in formation of local transient velocity disparities in the Se sublattice. The local differences in Se-phonon amplitudes result in noncompensated shear forces between the layers. This is an example of a multistep coherent launching mechanism. The energy of the optically excited electronic state dissipates energy into modes of the PLD through strong electron-phonon coupling. The rapid suppression of the PLD launches the third step, a coherent vibrational shear mode with low dissipation. The results highlight the importance in considering the 3D nature of the CDWs in the analysis of both structure and dynamics in transition-metal dichalcogenides.

Computational Methods for Charge Density Waves in 2D Materials

“…Sometimes confined systems, such as these 2D CDW materials, are subjected to conditions that may bring about a 3D-like nature. Such was the case in Ji et al [ 166 ], who reported on the optical suppression of the C-CDW over a sub-ps timescale. The group claims that the short timescales involved in establishing the stacking order implies that the nucleation of the IC-CDW phase is inherently of a 3D nature.…”

“…The simulated diffraction patterns are shown along [001] ( e ) and [102] ( h ). Reference [ 166 ] is an open-access article distributed under the terms of the Creative Commons CC BY ( (accessed on 14 December 2021)) license, which permits unrestricted use, distribution, and reproduction in any medium.…”

Coherent Phonon Disruption and Lock-In During a Photoinduced Charge-Density-Wave Phase Transition

“…Interestingly, observation of CAP d-spacing oscillations (Fig. 3c) is uncommon despite PLDs having large-amplitude LA-mode character consisting of significant basal-plane atomic modulations (8,40,(61)(62)(63)(64)(65). As seen in Figure 3c, both Bragg-scattering parameters display anomalous behavior for t < ~75 ps.…”

Coherent Phonon Disruption and Lock-In During a Photoinduced Charge-Density-Wave Phase Transition

“…3c) is uncommon despite PLDs having large-amplitude LA-mode character consisting of significant basal-plane atomic modulations. 8,40,55,[63][64][65][66] Despite this, subpicometer d-spacing changes are indeed generally observable with UEM. 40,67,68 Most interestingly, as seen in Figure 3c, both Bragg-scattering parameters display anomalous behaviors for t < ~75 ps.…”