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Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering

Samuel W. Teitelbaum1,2,*, Thomas C. Henighan1,3, Hanzhe Liu1,3, Mason P. Jiang1,3, Diling Zhu4, Matthieu Chollet4, Takahiro Sato4, Éamonn D. Murray5, Stephen Fahy6,7 et al.

Shane O'Mahony6,7, Trevor P. Bailey8, Ctirad Uher8, Mariano Trigo1,2, and David A. Reis1,2

  • 1Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
  • 2Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
  • 3Department of Physics, Stanford University, Stanford, California 94305, USA
  • 4Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
  • 5Department of Physics and Department of Materials, Imperial College London, London SW7 2AZ, United Kingdom
  • 6Tyndall National Institute, Cork T12 R5CP, Ireland
  • 7Department of Physics, University College Cork, Cork T12 R5CP, Ireland
  • 8Department of Physics, University of Michigan, Ann Arbor, Michigan 48109, USA

  • *Present address: Department of Physics, Arizona State University, Tempe, AZ 85287, USA, SamuelT@asu.edu
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Phys. Rev. B 103, L180101 – Published 18 May, 2021

DOI: https://doi.org/10.1103/PhysRevB.103.L180101

Abstract

We demonstrate an experimental approach to determining the excited-state interatomic forces using femtosecond x-ray pulses from an x-ray free-electron laser. We determine experimentally the excited-state interatomic forces that connect photoexcited carriers to the nonequilibrium lattice dynamics in the prototypical Peierls-distorted material, bismuth. The forces are obtained by a constrained least-squares fit of a pairwise interatomic force model to the excited-state phonon dispersion relation as measured by the time- and momentum-resolved x-ray diffuse scattering. We find that photoexcited carriers weaken predominantly the nearest-neighbor forces, which drives the measured softening of the transverse acoustic modes throughout the Brillouin zone as well as the zone-center A1g optical mode. This demonstrates a bond-selective approach to measuring electron-phonon coupling relevant to a broad range of photoinduced phase transitions and transient light-driven states in quantum materials.

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Phys. Rev. B 103, L180101– Published 18 May, 2021
  • Received 26 January 2021
  • Accepted 23 April 2021
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