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

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dc.contributor.authorTeitelbaum, Samuel W.
dc.contributor.authorHenighan, Thomas C.
dc.contributor.authorLiu, Hanzhe
dc.contributor.authorJiang, Mason P.
dc.contributor.authorZhu, Diling
dc.contributor.authorChollet, Matthieu
dc.contributor.authorSato, Takahiro
dc.contributor.authorMurray, Éamonn D.
dc.contributor.authorFahy, Stephen B.
dc.contributor.authorO'Mahony, Shane
dc.contributor.authorBailey, Trevor P.
dc.contributor.authorUher, Ctirad
dc.contributor.authorTrigo, Mariano
dc.contributor.authorReis, David A.
dc.contributor.funderScience Foundation Irelanden
dc.contributor.funderIrish Research Councilen
dc.contributor.funderOffice of Scienceen
dc.contributor.funderU.S. Department of Energyen
dc.contributor.funderBasic Energy Sciencesen
dc.contributor.funderDivision of Materials Sciences and Engineeringen
dc.date.accessioned2021-12-07T16:39:02Z
dc.date.available2021-12-07T16:39:02Z
dc.date.issued2021-05-18
dc.description.abstractWe 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.en
dc.description.sponsorshipDivision of Materials Sciences and Engineering (Contract No. DE-AC02-76SF00515); U.S. Department of Energy, Office of Basic Energy Sciences (Award No. DE-SC-0008574); Irish Research Council (Award No. GOIPG/2015/2784)en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.articleidL180101en
dc.identifier.citationTeitelbaum, S. W., Henighan, T. C., Liu, H., Jiang, M. P., Zhu, D., Chollet, M., Sato, T., Murray, E. D., Fahy, S. B., O’Mahony, S., Bailey, T. P., Uher, C., Trigo, M. and Reis, D. A. (2021) 'Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering', Physical Review B, 103(3), L180101 (6pp). doi: 10.1103/PhysRevB.103.L180101en
dc.identifier.doi10.1103/PhysRevB.103.L180101en
dc.identifier.eissn1550-235X
dc.identifier.endpage6en
dc.identifier.issn1098-0121
dc.identifier.issued3en
dc.identifier.journaltitlePhysical review B: Condensed matter and materials physicsen
dc.identifier.startpage1en
dc.identifier.urihttps://hdl.handle.net/10468/12328
dc.identifier.volume103en
dc.language.isoenen
dc.publisherAmerican Physical Societyen
dc.relation.projectinfo:eu-repo/grantAgreement/SFI/SFI Investigator Programme/12/IA/1601/IE/Ultrafast energy dissipation in semimetals and semiconductors: Simulation based on first-principles electronic structure theory/en
dc.rights© 2021, American Physical Society. All rights reserved.en
dc.subjectElectron-phonon couplingen
dc.subjectPeierls transitionen
dc.subjectPhononsen
dc.subjectStructural phase transitionen
dc.subjectUltrafast opticsen
dc.subjectX-ray scatteringen
dc.subjectX-ray lasersen
dc.subjectNonequilibrium systemsen
dc.subjectSemimetalsen
dc.subjectSynchrotron radiation & free-electron lasersen
dc.subjectPhotoexcitationen
dc.subjectUltrafast pump-probe spectroscopyen
dc.titleMeasurements of nonequilibrium interatomic forces using time-domain x-ray scatteringen
dc.typeArticle (peer-reviewed)en
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