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  • Letter

Unveiling the underlying interactions in Ta2NiSe5 from photoinduced lifetime change

Denis Golež1,2,3,*, Sydney K. Y. Dufresne4,5,*, Min-Jae Kim6,7,8, Fabio Boschini4,5,9, Hao Chu4,5,6, Yuta Murakami10, Giorgio Levy4,5, Arthur K. Mills4,5, Sergey Zhdanovich4,5 et al.

Masahiko Isobe6, Hidenori Takagi6,10, Stefan Kaiser6,7,8, Philipp Werner11, David J. Jones4,5, Antoine Georges3,12,13,14, Andrea Damascelli4,5, and Andrew J. Millis3,15

  • 1Jozef Stefan Institute, Jamova 39, SI-1000 Ljubljana, Slovenia
  • 2Faculty of Mathematics and Physics, University of Ljubljana, Jadranska 19, SI-1000 Ljubljana, Slovenia
  • 3Center for Computational Quantum Physics, Flatiron Institute, 162 Fifth Avenue, New York, New York 10010, USA
  • 4Quantum Matter Institute, University of British Columbia, Vancouver, British Columbia, Canada V6T 1Z4
  • 5Department of Physics & Astronomy, University of British Columbia, Vancouver, British Columbia, Canada V6T 1Z1
  • 6Max Planck Institute for Solid State Research, Heisenbergstrasse 1, D-70569 Stuttgart, Germany
  • 74th Physics Institute, University of Stuttgart, D-70569 Stuttgart, Germany
  • 8Institut für Festkörper- und Materialphysik, Technische Universität Dresden, D-01069 Dresden, Germany
  • 9Centre Énergie Matériaux Télécommunications, Institut National de la Recherche Scientifique, Varennes, Québec, Canada J3X 1S2
  • 10Department of Physics, Tokyo Institute of Technology, Meguro, Tokyo 152-8551, Japan
  • 11Department of Physics, University of Fribourg, CH-1700 Fribourg, Switzerland
  • 12Collège de France, 11 place Marcelin Berthelot, F-75005 Paris, France
  • 13CPHT, CNRS, Ecole Polytechnique, IP Paris, F-91128 Palaiseau, France
  • 14Department of Quantum Matter Physics, University of Geneva, CH-1211 Geneva 4, Switzerland
  • 15Department of Physics, Columbia University, 538 West 120th Street, New York, New York 10027, USA

  • *These authors contributed equally to this work.

Phys. Rev. B 106, L121106 – Published 14 September, 2022

DOI: https://doi.org/10.1103/PhysRevB.106.L121106

Abstract

We present a generic procedure for quantifying the interplay of electronic and lattice degrees of freedom in photodoped insulators through a comparative analysis of theoretical many-body simulations and time- and angle-resolved photoemission spectroscopy (TR-ARPES) of the transient response of the candidate excitonic insulator Ta2NiSe5. Our analysis demonstrates that the electron-electron interactions dominate the electron-phonon ones. In particular, a detailed analysis of the TR-ARPES spectrum enables a clear separation of the dominant broadening (electronic lifetime) effects from the much smaller band-gap renormalization. Theoretical calculations show that the observed strong spectral broadening arises from the electronic scattering of the photoexcited particle-hole pairs and cannot be accounted for in a model in which electron-phonon interactions are dominant. The competing interactions were quantified using the scaling analysis in the weak fluence regime. We demonstrate that the magnitude of the weaker subdominant band-gap renormalization sensitively depends on the distance from the semiconductor/semimetal transition in the high-temperature state, which could explain the apparent contradictions between various TR-ARPES experiments. The analysis presented here indicates that electron-electron interactions play a vital role (albeit not the sole one) in stabilizing the insulating state, and establishes the comparison between lifetime and gap evolution as an important probe of correlated insulators.

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