Real-time observation of the coherent transition to a metastable emergent state in 1T-TaS$_2$

TL;DR

This paper demonstrates real-time observation of a rapid electronic transition to a metastable state in 1T-TaS2 using femtosecond spectroscopy, revealing ultrafast coherent switching and lattice relaxation dynamics.

Contribution

It provides the first real-time measurement of the ultrafast electronic and lattice dynamics during the transition to a metastable state in 1T-TaS2, highlighting a topological electronic transition.

Findings

Coherent switching of collective mode frequency occurs in 400 fs.

Electronic band structure transforms within 300 fs.

Lattice relaxation occurs over 4.7 ps.

Abstract

The transition to a hidden metastable state in 1T-TaS2 is investigated in real time using coherent time-resolved femtosecond spectroscopy. Relying on spectral differences between phonon modes in the equilibrium states and in the metastable state, and temperature-tuning the metastable state lifetime, we perform stroboscopic measurements of the electronic response and switching of coherent oscillation frequency through the transition. Very fast coherent switching of the collective mode frequency is observed (400 fs), comparable to the electronic timescale (300 fs). A slower, 4.7 ps process is attributed to lattice relaxation. The observations are described well by a fast electronic band structure transformation into the metastable state, consistent with a topological transition.