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

Abstract

Here, 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.

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [3];  [3];  [3];  [4];  [5];  [5]; ORCiD logo [6];  [6];  [3]; ORCiD logo [3]
+ Show Author Affiliations
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Arizona State Univ., Tempe, AZ (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Imperial College, London (United Kingdom)
  5. Tyndall National Inst., Cork (Ireland); Univ. College, Cork (Ireland)
  6. Univ. of Michigan, Ann Arbor, MI (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Science Foundation Ireland; Irish Research Council Award
OSTI Identifier:
1808597
Grant/Contract Number:  
SC-0008574; AC02-76SF00515; 12/IA/1601; GOIPG/2015/2784
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 103; Journal Issue: 18; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; electron-phonon coupling; Peierls transition; phonons; structural phase transition; ultrafast optics; x-ray lasers; nonequilibrium systems; semimetals; synchrotron radiation & free-electron lasers; photoexcitation; ultrafast pump-probe spectroscopy; x-ray scattering

Citation Formats

Teitelbaum, Samuel W., Henighan, Thomas C., Liu, Hanzhe, Jiang, Mason P., Zhu, Diling, Chollet, Matthieu, Sato, Takahiro, Murray, Éamonn D., Fahy, Stephen, O'Mahony, Shane, Bailey, Trevor P., Uher, Ctirad, Trigo, Mariano, and Reis, David A. Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering. United States: N. p., 2021. Web. doi:10.1103/physrevb.103.l180101.
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Teitelbaum, Samuel W., Henighan, Thomas C., Liu, Hanzhe, Jiang, Mason P., Zhu, Diling, Chollet, Matthieu, Sato, Takahiro, Murray, Éamonn D., Fahy, Stephen, O'Mahony, Shane, Bailey, Trevor P., Uher, Ctirad, Trigo, Mariano, & Reis, David A. Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering. United States. https://doi.org/10.1103/physrevb.103.l180101
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Teitelbaum, Samuel W., Henighan, Thomas C., Liu, Hanzhe, Jiang, Mason P., Zhu, Diling, Chollet, Matthieu, Sato, Takahiro, Murray, Éamonn D., Fahy, Stephen, O'Mahony, Shane, Bailey, Trevor P., Uher, Ctirad, Trigo, Mariano, and Reis, David A. Tue . "Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering". United States. https://doi.org/10.1103/physrevb.103.l180101. https://www.osti.gov/servlets/purl/1808597.
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@article{osti_1808597,
title = {Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering},
author = {Teitelbaum, Samuel W. and Henighan, Thomas C. and Liu, Hanzhe and Jiang, Mason P. and Zhu, Diling and Chollet, Matthieu and Sato, Takahiro and Murray, Éamonn D. and Fahy, Stephen and O'Mahony, Shane and Bailey, Trevor P. and Uher, Ctirad and Trigo, Mariano and Reis, David A.},
abstractNote = {Here, 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.},
doi = {10.1103/physrevb.103.l180101},
journal = {Physical Review B},
number = 18,
volume = 103,
place = {United States},
year = {Tue May 18 00:00:00 EDT 2021},
month = {Tue May 18 00:00:00 EDT 2021}
}
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https://doi.org/10.1103/physrevb.103.l180101
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