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.

References in corpus (7)

• Terahertz-Field-Induced Ferroelectricity in Quantum Paraelectric SrTiO${}_3$
• Optical detection and manipulation of spontaneous gyrotropic electronic order in a transition-metal dichalcogenide semimetal
• Ultrafast electron calorimetry uncovers a new long-lived metastable state in 1T-TaSe${}_2$ mediated by mode-selective electron-phonon coupling
• Photoinduced multistage phase transitions in Ta2NiSe5
• A time-domain phase diagram of metastable states in a charge ordered quantum material
• Zoology of domain walls in quasi-2D correlated charge density wave of 1T-TaS2
• Role of equilibrium fluctuations in light-induced order

Cited by in corpus (13)

• Terahertz field-driven magnon upconversion in an antiferromagnet
• Mott materials: unsuccessful metals with a bright future
• Optical-pump terahertz-probe spectroscopy in high magnetic fields with kHz single-shot detection
• Ultrafast generation of hidden phases via energy-tuned electronic photoexcitation in magnetite
• Distinguishing and controlling Mottness in 1T-TaS${}_2$ by ultrafast light
• Mott resistive switching initiated by topological defects
• Dynamic phase transition into a mixed-CDW state in 1$T$-TaS${}_2$ via a thermal quench
• Fate of transient order parameter domain walls in ultrafast experiments
• Switching of an antiferromagnet controlled by spin canting in a laser-induced hidden phase
• Uncovering the nature of transient and metastable non-equilibrium phases in 1$T$-TaS${}_2$
• Electromagnon signatures of a metastable multiferroic state
• Excitations across the equilibrium and photoinduced `hidden' states of magnetoresistive manganites
• Ultrafast non-thermal suppression of ferroelectricity by carrier screening in LiNbO3