Snapshots of a light-induced metastable hidden phase driven by the collapse of charge order

Abstract

Nonequilibrium hidden states, both transient and long-lived, provide a unique window into thermally inaccessible regimes of strong coupling between microscopic degrees of freedom in quantum materials. Understanding the physical origin of these states is of both fundamental and practical significance, allowing the exploration of far-from-equilibrium thermodynamics and the development of optoelectronic devices with on-demand photoresponses. However, mapping the ultrafast formation of a long-lived hidden phase remains a long-standing challenge in physics since the initial state of the system is not recovered rapidly and conventional pump-probe methods are thus not applicable. Here, using a suite of state-of-the-art single-shot spectroscopy techniques, we present a direct ultrafast visualization of the photoinduced phase transition to both transient and long-lived hidden states in an electronic crystal, 1T-TaS2. Capturing the dynamics of this complex phase transformation in a single-shot fashion demonstrates a commonality in microscopic pathways, driven by the collapse of charge order, that the system undergoes to enter the hidden state and provides unambiguous spectral fingerprints that distinguish such state from thermally accessible phases. We present a theory of fluctuation-dominated process that explains both the dynamics and the nature of the metastable state. Our results settle the debate around the origin of this elusive metastable state and pave the way for the discovery of new quantum phases of matter.