Snapshots of a light-induced metastable hidden phase driven by the collapse of charge order
Abstract
Nonequilibrium hidden states provide a unique window into thermally inaccessible regimes of strong coupling between microscopic degrees of freedom in quantum materials. Understanding the origin of these states allows 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 longstanding challenge since the initial state is not recovered rapidly. Here, using 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, and demonstrate a commonality in their microscopic pathways, driven by the collapse of charge order. We present a theory of fluctuation-dominated process that helps explain the nature of the metastable state. Our results shed light on the origin of this elusive state and pave the way for the discovery of other exotic phases of matter.
Copyright and License
© 2022 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).
Acknowledgement
We thank J. Zhu for helping with the samples and for useful discussions.
Funding
This work was supported by U.S. Department of Energy, Office of Basic Energy Sciences, award no. DE-SC0019126 (F.Y.G., Z.Z., Y.-H.C., Z.-J.L., and K.A.N.); Gordon and Betty Moore Foundation EPiQS Initiative grant GBMF3848 (L.Y. and J.G.C.); Gordon and Betty Moore Foundation EPiQS Initiative grant GBMF9070 (L.Y. and J.G.C.); Harvard Quantum Initiative, Postdoctoral Fellowship in Quantum Science and Engineering (Z.S.). Robert A. Welch Foundation, award no. F-2092-20220331 (E.B.).
Contributions
F.Y.G. and Z.Z. conceived of the study. F.Y.G. and Z.Z. performed all the experiments with support from Y.-H.C. and Z.-J.L.; L.Y. synthesized the samples under the supervision of J.G.C.; Z.S. provided the theoretical interpretation. F.Y.G., Z.Z., and E.B. analyzed the data and led the manuscript preparation; K.A.N. and E.B. supervised the project.
Data Availability
All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials.
Conflict of Interest
The authors declare that they have no competing interests.
Attached Files
sciadv.abp9076.pdf: Published article
sciadv.abp9076_sm.pdf : Supplementary information
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Additional details
- PMCID
- PMC9307249
- United States Department of Energy
- DE-SC0019126
- Gordon and Betty Moore Foundation
- GBMF3848
- Gordon and Betty Moore Foundation
- GBMF9070
- Harvard University
- Welch Foundation
- F-2092-20220331
- Accepted
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2022-06-09