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    Role of Equilibrium Fluctuations in Light-Induced Order

    Alfred Zong1,2,*, Pavel E. Dolgirev3,*, Anshul Kogar1,4,*, Yifan Su1, Xiaozhe Shen5, Joshua A. W. Straquadine6,7,8, Xirui Wang1, Duan Luo5, Michael E. Kozina5 et al.

    Alexander H. Reid5, Renkai Li5, Jie Yang5, Stephen P. Weathersby5, Suji Park5,9, Edbert J. Sie7,8, Pablo Jarillo-Herrero1, Ian R. Fisher6,7,8, Xijie Wang5, Eugene Demler3,10, and Nuh Gedik1,†

    • 1Department of Physics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
    • 2Department of Chemistry, University of California at Berkeley, Berkeley, California 94720, USA
    • 3Department of Physics, Harvard University, Cambridge, Massachusetts 02138, USA
    • 4Department of Physics and Astronomy, University of California at Los Angeles, Los Angeles, California 90095, USA
    • 5SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
    • 6Department of Applied Physics, Stanford University, Stanford, California 94305, USA
    • 7SIMES, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
    • 8Geballe Laboratory for Advanced Materials, Stanford University, Stanford, California 94305, USA
    • 9Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, USA
    • 10Institute for Theoretical Physics, ETH Zurich, 8093 Zurich, Switzerland

    • *These authors contributed equally to this work.
    • †Corresponding author. gedik@mit.edu
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    Phys. Rev. Lett. 127, 227401 – Published 24 November, 2021

    DOI: https://doi.org/10.1103/PhysRevLett.127.227401

    Abstract

    Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are “hidden” under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host hidden orders after laser excitation.

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    Phys. Rev. Lett. 127, 227401– Published 24 November, 2021
    • Received 2 March 2021
    • Accepted 1 October 2021
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