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Title: Thickness-dependent electron–lattice equilibration in laser-excited thin bismuth films

Abstract

Electron–phonon coupling processes determine electronic transport properties of materials and are responsible for the transfer of electronic excess energy to the lattice. With decreasing device dimensions an understanding of these processes in nanoscale materials is becoming increasingly important. We use time-resolved electron diffraction to directly study energy relaxation in thin bismuth films after optical excitation. Precise measurements of the transient Debye–Waller-effect for various film thicknesses and over an extended range of excitation fluences allow to separate different contributions to the incoherent lattice response. While phonon softening in the electronically excited state is responsible for an immediate increase of the r.m.s. atomic displacement within a few hundred fs, 'ordinary' electron–phonon coupling leads to subsequent heating of the material on a few ps time-scale. Moreover, the data reveal distinct changes in the energy transfer dynamics which becomes faster for stronger excitation and smaller film thickness, respectively. The latter effect is attributed to a cross-interfacial coupling of excited electrons to phonons in the substrate.

Authors:
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Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1238985
Alternate Identifier(s):
OSTI ID: 1237587; OSTI ID: 1238989
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Published Article
Journal Name:
New Journal of Physics
Additional Journal Information:
Journal Name: New Journal of Physics Journal Volume: 17 Journal Issue: 11; Journal ID: ISSN 1367-2630
Publisher:
IOP Publishing
Country of Publication:
United Kingdom
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; electron-phonon coupling; bismuth; thin films; time-resolved electron diffraction

Citation Formats

Sokolowski-Tinten, K., Li, R. K., Reid, A. H., Weathersby, S. P., Quirin, F., Chase, T., Coffee, R., Corbett, J., Fry, A., Hartmann, N., Hast, C., Hettel, R., Hoegen, M. Horn von, Janoschka, D., Lewandowski, J. R., Ligges, M., Heringdorf, F. Meyer zu, Shen, X., Vecchione, T., Witt, C., Wu, J., Dürr, H. A., and Wang, X. J. Thickness-dependent electron–lattice equilibration in laser-excited thin bismuth films. United Kingdom: N. p., 2015. Web. doi:10.1088/1367-2630/17/11/113047.
Sokolowski-Tinten, K., Li, R. K., Reid, A. H., Weathersby, S. P., Quirin, F., Chase, T., Coffee, R., Corbett, J., Fry, A., Hartmann, N., Hast, C., Hettel, R., Hoegen, M. Horn von, Janoschka, D., Lewandowski, J. R., Ligges, M., Heringdorf, F. Meyer zu, Shen, X., Vecchione, T., Witt, C., Wu, J., Dürr, H. A., & Wang, X. J. Thickness-dependent electron–lattice equilibration in laser-excited thin bismuth films. United Kingdom. doi:10.1088/1367-2630/17/11/113047.
Sokolowski-Tinten, K., Li, R. K., Reid, A. H., Weathersby, S. P., Quirin, F., Chase, T., Coffee, R., Corbett, J., Fry, A., Hartmann, N., Hast, C., Hettel, R., Hoegen, M. Horn von, Janoschka, D., Lewandowski, J. R., Ligges, M., Heringdorf, F. Meyer zu, Shen, X., Vecchione, T., Witt, C., Wu, J., Dürr, H. A., and Wang, X. J. Sun . "Thickness-dependent electron–lattice equilibration in laser-excited thin bismuth films". United Kingdom. doi:10.1088/1367-2630/17/11/113047.
@article{osti_1238985,
title = {Thickness-dependent electron–lattice equilibration in laser-excited thin bismuth films},
author = {Sokolowski-Tinten, K. and Li, R. K. and Reid, A. H. and Weathersby, S. P. and Quirin, F. and Chase, T. and Coffee, R. and Corbett, J. and Fry, A. and Hartmann, N. and Hast, C. and Hettel, R. and Hoegen, M. Horn von and Janoschka, D. and Lewandowski, J. R. and Ligges, M. and Heringdorf, F. Meyer zu and Shen, X. and Vecchione, T. and Witt, C. and Wu, J. and Dürr, H. A. and Wang, X. J.},
abstractNote = {Electron–phonon coupling processes determine electronic transport properties of materials and are responsible for the transfer of electronic excess energy to the lattice. With decreasing device dimensions an understanding of these processes in nanoscale materials is becoming increasingly important. We use time-resolved electron diffraction to directly study energy relaxation in thin bismuth films after optical excitation. Precise measurements of the transient Debye–Waller-effect for various film thicknesses and over an extended range of excitation fluences allow to separate different contributions to the incoherent lattice response. While phonon softening in the electronically excited state is responsible for an immediate increase of the r.m.s. atomic displacement within a few hundred fs, 'ordinary' electron–phonon coupling leads to subsequent heating of the material on a few ps time-scale. Moreover, the data reveal distinct changes in the energy transfer dynamics which becomes faster for stronger excitation and smaller film thickness, respectively. The latter effect is attributed to a cross-interfacial coupling of excited electrons to phonons in the substrate.},
doi = {10.1088/1367-2630/17/11/113047},
journal = {New Journal of Physics},
number = 11,
volume = 17,
place = {United Kingdom},
year = {2015},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1088/1367-2630/17/11/113047

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Cited by: 6 works
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Works referenced in this record:

Optical Probing of Ultrafast Electronic Decay in Bi and Sb with Slow Phonons
journal, January 2013


Study of the Electron–Phonon Relaxation in Thin Metal Films Using Transient Thermoreflectance Technique
journal, August 2011

  • Ma, Weigang; Wang, Haidong; Zhang, Xing
  • International Journal of Thermophysics, Vol. 34, Issue 12
  • DOI: 10.1007/s10765-011-1063-2

Ultrasonic studies on bismuth single crystals
journal, March 1975


Time- and momentum-resolved probe of heat transport in photo-excited bismuth
journal, May 2013

  • Chen, J.; Trigo, M.; Fahy, S.
  • Applied Physics Letters, Vol. 102, Issue 18
  • DOI: 10.1063/1.4804291

Coherent phonons in bismuth film observed by ultrafast electron diffraction
journal, March 2011

  • Bugayev, A.; Esmail, A.; Abdel-Fattah, M.
  • AIP Advances, Vol. 1, Issue 1
  • DOI: 10.1063/1.3574888

Directly Observing Squeezed Phonon States with Femtosecond X-Ray Diffraction
journal, April 2009


Carrier Relaxation and Lattice Heating Dynamics in Silicon Revealed by Femtosecond Electron Diffraction
journal, December 2006

  • Harb, Maher; Ernstorfer, Ralph; Dartigalongue, Thibault
  • The Journal of Physical Chemistry B, Vol. 110, Issue 50
  • DOI: 10.1021/jp064649n

The surfaces of bismuth: Structural and electronic properties
journal, January 2006


Comparing ultrafast surface and bulk heating using time-resolved electron diffraction
journal, April 2014

  • Streubühr, C.; Kalus, A.; Zhou, P.
  • Applied Physics Letters, Vol. 104, Issue 16
  • DOI: 10.1063/1.4872055

Fourier-transform inelastic X-ray scattering from time- and momentum-dependent phonon–phonon correlations
journal, October 2013

  • Trigo, M.; Fuchs, M.; Chen, J.
  • Nature Physics, Vol. 9, Issue 12
  • DOI: 10.1038/nphys2788

Electron-phonon coupling and electron heat capacity of metals under conditions of strong electron-phonon nonequilibrium
journal, February 2008


Heat Transfer Across Metal-Dielectric Interfaces During Ultrafast-Laser Heating
journal, February 2012

  • Guo, Liang; Hodson, Stephen L.; Fisher, Timothy S.
  • Journal of Heat Transfer, Vol. 134, Issue 4
  • DOI: 10.1115/1.4005255

Superconductivity above 100 K in single-layer FeSe films on doped SrTiO3
journal, November 2014

  • Ge, Jian-Feng; Liu, Zhi-Long; Liu, Canhua
  • Nature Materials, Vol. 14, Issue 3
  • DOI: 10.1038/nmat4153

High-quality epitaxial Bi(111) films on Si(111) by isochronal annealing
journal, September 2012


Experimental study of electron-phonon coupling and electron internal thermalization in epitaxially grown ultrathin copper films
journal, January 2015


Semimetal-to-semiconductor transition in bismuth thin films
journal, October 1993


Oscillatory electron-phonon coupling in ultra-thin silver films on V(100)
journal, June 2000


Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit
journal, March 2003

  • Sokolowski-Tinten, Klaus; Blome, Christian; Blums, Juris
  • Nature, Vol. 422, Issue 6929
  • DOI: 10.1038/nature01490

Electronic Kapitza conductance at a diamond-Pb interface
journal, August 1994


Electron Diffraction Studies of Structural Dynamics of Bismuth Nanoparticles
journal, April 2013

  • Esmail, Ahmed R.; Bugayev, Aleksey; Elsayed-Ali, Hani E.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 17
  • DOI: 10.1021/jp401902t

Interfacial mode coupling as the origin of the enhancement of Tc in FeSe films on SrTiO3
journal, November 2014

  • Lee, J. J.; Schmitt, F. T.; Moore, R. G.
  • Nature, Vol. 515, Issue 7526
  • DOI: 10.1038/nature13894

Thermal boundary conductance in heterostructures studied by ultrafast electron diffraction
journal, September 2006


Anisotropic response of nanosized bismuth films upon femtosecond laser excitation monitored by ultrafast electron diffraction
journal, October 2011

  • Esmail, Ahmed R.; Elsayed-Ali, Hani E.
  • Applied Physics Letters, Vol. 99, Issue 16
  • DOI: 10.1063/1.3652919

Mechanism of coherent acoustic phonon generation under nonequilibrium conditions
journal, September 2005


Transient (000)-order attenuation effects in ultrafast transmission electron diffraction
journal, March 2011

  • Ligges, Manuel; Rajković, Ivan; Streubühr, Carla
  • Journal of Applied Physics, Vol. 109, Issue 6
  • DOI: 10.1063/1.3554405

Parameterization of the temperature dependence of the Debye–Waller factors
journal, September 1999

  • Gao, H. X.; Peng, L. -M.
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 55, Issue 5
  • DOI: 10.1107/S0108767399005176

Laser-induced phonon-phonon interactions in bismuth
journal, December 2006

  • Zijlstra, Eeuwe S.; Tatarinova, Larisa L.; Garcia, Martin E.
  • Physical Review B, Vol. 74, Issue 22
  • DOI: 10.1103/PhysRevB.74.220301

Direct observation of non-fully-symmetric coherent optical phonons by femtosecond x-ray diffraction
journal, February 2013


Large Electron-Phonon Coupling at an Interface
journal, June 2002


Excitation of longitudinal and transverse coherent acoustic phonons in nanometer free-standing films of (001) Si
journal, March 2009


Debye-Waller factor and thermal expansion of arsenic, antimony and bismuth
journal, March 1978

  • Fischer, P.; Sosnowska, I.; Szymanski, M.
  • Journal of Physics C: Solid State Physics, Vol. 11, Issue 6
  • DOI: 10.1088/0022-3719/11/6/011

Effect of Intense Laser Irradiation on the Lattice Stability of Semiconductors and Metals
journal, February 2006


Electronic acceleration of atomic motions and disordering in bismuth
journal, March 2009

  • Sciaini, Germán; Harb, Maher; Kruglik, Sergei G.
  • Nature, Vol. 458, Issue 7234
  • DOI: 10.1038/nature07788

Dynamics of Coherent Anharmonic Phonons in Bismuth Using High Density Photoexcitation
journal, January 2002


Electronic Kapitza conductance due to inelastic electron-boundary scattering
journal, October 1998


Observation of ultrafast lattice heating using time resolved electron diffraction
journal, March 2009

  • Ligges, M.; Rajkovic, I.; Zhou, P.
  • Applied Physics Letters, Vol. 94, Issue 10
  • DOI: 10.1063/1.3095497

Transport Properties of Bismuth Single Crystals
journal, January 1963

  • Gallo, C. F.; Chandrasekhar, B. S.; Sutter, P. H.
  • Journal of Applied Physics, Vol. 34, Issue 1
  • DOI: 10.1063/1.1729056

Phonon confinement effects in ultrathin epitaxial bismuth films on silicon studied by time-resolved electron diffraction
journal, July 2009


Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory
journal, July 2015

  • Weathersby, S. P.; Brown, G.; Centurion, M.
  • Review of Scientific Instruments, Vol. 86, Issue 7
  • DOI: 10.1063/1.4926994

Electron Cooling and Debye-Waller Effect in Photoexcited Bismuth
journal, January 2013


X-ray study of Bi, Sb and Bi1-x-Sbx alloys
journal, November 2005

  • Shankar Narayana, M.; Gopi Krishna, N.
  • physica status solidi (a), Vol. 202, Issue 14
  • DOI: 10.1002/pssa.200520090

Influence of the electron–phonon interfacial conductance on the thermal transport at metal/dielectric interfaces
journal, November 2014


Nanoscale Depth-Resolved Coherent Femtosecond Motion in Laser-Excited Bismuth
journal, April 2008


Dynamics and coherent control of high-amplitude optical phonons in bismuth
journal, August 2001

  • DeCamp, M. F.; Reis, D. A.; Bucksbaum, P. H.
  • Physical Review B, Vol. 64, Issue 9, Article No. 092301
  • DOI: 10.1103/PhysRevB.64.092301

Relaxation dynamics in laser-excited metals under nonequilibrium conditions
journal, January 2013


Nonuniformity in lattice contraction of bismuth nanoclusters heated near its melting point
journal, April 2011

  • Esmail, A.; Abdel-Fattah, M.; Elsayed-Ali, H. E.
  • Journal of Applied Physics, Vol. 109, Issue 8
  • DOI: 10.1063/1.3565028

Optical Studies of Dynamics in Noble Metal Nanostructures
journal, June 2011


Electron and lattice dynamics following optical excitation of metals
journal, January 2000


Evidence of enhanced electron-phonon coupling in ultrathin epitaxial copper films
journal, November 2013

  • Timalsina, Yukta P.; Shen, Xiaohan; Boruchowitz, Grant
  • Applied Physics Letters, Vol. 103, Issue 19
  • DOI: 10.1063/1.4829643

First-Principles Calculation of Femtosecond Symmetry-Breaking Atomic Forces in Photoexcited Bismuth
journal, February 2015


Optical properties of pulsed laser deposited bismuth films
journal, December 1996

  • de Sande, J. C. G.; Missana, T.; Afonso, C. N.
  • Journal of Applied Physics, Vol. 80, Issue 12
  • DOI: 10.1063/1.363775

Squeezed Thermal Phonons Precurse Nonthermal Melting of Silicon as a Function of Fluence
journal, January 2013


Ultrafast Bond Softening in Bismuth: Mapping a Solid's Interatomic Potential with X-rays
journal, February 2007


Coherent THz Phonons Driven by Light Pulses and the Sb Problem: What is the Mechanism?
journal, October 1996


Ultrafast and steady-state laser heating effects on electron relaxation and phonon coupling mechanisms in thin gold films
journal, November 2013

  • Hopkins, Patrick E.; Duda, John C.; Kaehr, Bryan
  • Applied Physics Letters, Vol. 103, Issue 21
  • DOI: 10.1063/1.4833415

Measurement of the electron-phonon coupling factor dependence on film thickness and grain size in Au, Cr, and Al
journal, January 1999

  • Hostetler, John L.; Smith, Andrew N.; Czajkowsky, Daniel M.
  • Applied Optics, Vol. 38, Issue 16
  • DOI: 10.1364/AO.38.003614

Temperature factors of polycrystalline arsenic, antimony and bismuth in the low-temperature range
journal, April 1975

  • Sosnowska, I.; Fischer, P.; Wartburg, W. von
  • Journal of Physics C: Solid State Physics, Vol. 8, Issue 8
  • DOI: 10.1088/0022-3719/8/8/018

Bi(111) Thin Film with Insulating Interior but Metallic Surfaces
journal, October 2012


Phonon dispersion relations and softening in photoexcited bismuth from first principles
journal, May 2007


    Works referencing / citing this record:

    Optically excited structural transition in atomic wires on surfaces at the quantum limit
    journal, March 2017


    A direct electron detector for time-resolved MeV electron microscopy
    journal, March 2017

    • Vecchione, T.; Denes, P.; Jobe, R. K.
    • Review of Scientific Instruments, Vol. 88, Issue 3
    • DOI: 10.1063/1.4977923

    Electron-lattice energy relaxation in laser-excited thin-film Au-insulator heterostructures studied by ultrafast MeV electron diffraction
    journal, September 2017

    • Sokolowski-Tinten, K.; Shen, X.; Zheng, Q.
    • Structural Dynamics, Vol. 4, Issue 5
    • DOI: 10.1063/1.4995258

    Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure
    journal, November 2019


    Coherent and incoherent structural dynamics in laser-excited antimony
    journal, February 2017


    Femtosecond phase-transition in hard x-ray excited bismuth
    text, January 2019