Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure
Abstract
The element specificity of soft x-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. As such, using [Fe/MgO]$$_n$$ as a model system, we perform ultraviolet pump/soft x-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield comprehensive insight into the microscopic processes leading to local relaxation within a single constituent or nonlocal relaxation between two constituents. Besides electronic excitations in Fe, which are monitored at the Fe L3 absorption edge and relax within 1 ps by electron-phonon coupling, soft x-ray analysis identifies a change at the oxygen K absorption edge of theMgO layers which occurs within 0.5 ps. This ultrafast energy transfer across the Fe-MgO interface is mediated by high-frequency, interface vibrational modes, which are excited by hot electrons in Fe and couple to vibrations in MgO in a mode-selective, nonthermal manner. A second, slower timescale is identified at the oxygen K pre-edge and the Fe L3 edge. The slower process represents energy transfer by acoustic phonons and contributes to thermalization of the entire heterostructure. We thus find that the interfacial energy transfer is associated with nonequilibrium behavior in the phonon system. Because our experiments lack signatures of charge transfer across the interface, we conclude that phonon-mediated processes dominate the competition of electronic and lattice excitations in these nonlocal, nonequilibrium dynamics.
- Authors:
-
[1]
- Univ. of Duisburg-Essen (Germany). Center for Nanointegration Duisburg-Essen (CENIDE)
- Forschungszentrum Jülich (Germany). Peter-Grünberg-Inst.
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- Sponsoring Org.:
- German Research Foundation (DFG); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1596966
- Grant/Contract Number:
- 278162697; WE2623/13; INST-20876/209-1-FUGG; INST-20876/243-1-FUGG; AC02-05-CH11231; AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 100; Journal Issue: 17; 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; 36 MATERIALS SCIENCE
Citation Formats
Rothenbach, N., Gruner, M. E., Ollefs, K., Schmitz-Antoniak, C., Salamon, S., Zhou, P., Li, R., Mo, M., Park, S., Shen, X., Weathersby, S., Yang, J., Wang, X. J., Pentcheva, R., Wende, H., Bovensiepen, U., Sokolowski-Tinten, K., and Eschenlohr, A. Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure. United States: N. p., 2019.
Web. doi:10.1103/PhysRevB.100.174301.
Rothenbach, N., Gruner, M. E., Ollefs, K., Schmitz-Antoniak, C., Salamon, S., Zhou, P., Li, R., Mo, M., Park, S., Shen, X., Weathersby, S., Yang, J., Wang, X. J., Pentcheva, R., Wende, H., Bovensiepen, U., Sokolowski-Tinten, K., & Eschenlohr, A. Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure. United States. https://doi.org/10.1103/PhysRevB.100.174301
Rothenbach, N., Gruner, M. E., Ollefs, K., Schmitz-Antoniak, C., Salamon, S., Zhou, P., Li, R., Mo, M., Park, S., Shen, X., Weathersby, S., Yang, J., Wang, X. J., Pentcheva, R., Wende, H., Bovensiepen, U., Sokolowski-Tinten, K., and Eschenlohr, A. Tue .
"Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure". United States. https://doi.org/10.1103/PhysRevB.100.174301. https://www.osti.gov/servlets/purl/1596966.
@article{osti_1596966,
title = {Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure},
author = {Rothenbach, N. and Gruner, M. E. and Ollefs, K. and Schmitz-Antoniak, C. and Salamon, S. and Zhou, P. and Li, R. and Mo, M. and Park, S. and Shen, X. and Weathersby, S. and Yang, J. and Wang, X. J. and Pentcheva, R. and Wende, H. and Bovensiepen, U. and Sokolowski-Tinten, K. and Eschenlohr, A.},
abstractNote = {The element specificity of soft x-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. As such, using [Fe/MgO]$_n$ as a model system, we perform ultraviolet pump/soft x-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield comprehensive insight into the microscopic processes leading to local relaxation within a single constituent or nonlocal relaxation between two constituents. Besides electronic excitations in Fe, which are monitored at the Fe L3 absorption edge and relax within 1 ps by electron-phonon coupling, soft x-ray analysis identifies a change at the oxygen K absorption edge of theMgO layers which occurs within 0.5 ps. This ultrafast energy transfer across the Fe-MgO interface is mediated by high-frequency, interface vibrational modes, which are excited by hot electrons in Fe and couple to vibrations in MgO in a mode-selective, nonthermal manner. A second, slower timescale is identified at the oxygen K pre-edge and the Fe L3 edge. The slower process represents energy transfer by acoustic phonons and contributes to thermalization of the entire heterostructure. We thus find that the interfacial energy transfer is associated with nonequilibrium behavior in the phonon system. Because our experiments lack signatures of charge transfer across the interface, we conclude that phonon-mediated processes dominate the competition of electronic and lattice excitations in these nonlocal, nonequilibrium dynamics.},
doi = {10.1103/PhysRevB.100.174301},
journal = {Physical Review B},
number = 17,
volume = 100,
place = {United States},
year = {Tue Nov 05 00:00:00 EST 2019},
month = {Tue Nov 05 00:00:00 EST 2019}
}
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Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Role of interface disorder on thermal boundary conductance using a virtual crystal approach
journal, January 2007
- Beechem, Thomas; Graham, Samuel; Hopkins, Patrick
- Applied Physics Letters, Vol. 90, Issue 5
Thermal Boundary Conductance: A Materials Science Perspective
journal, July 2016
- Monachon, Christian; Weber, Ludger; Dames, Chris
- Annual Review of Materials Research, Vol. 46, Issue 1
Temperature Dependence of Debye-Waller Factors in bcc Metals. I
journal, December 1977
- Lal Kharoo, Hira; P. Gupta, O.; P. Hemkar, M.
- Journal of the Physical Society of Japan, Vol. 43, Issue 6
Energy dissipation from a correlated system driven out of equilibrium
journal, December 2016
- Rameau, J. D.; Freutel, S.; Kemper, A. F.
- Nature Communications, Vol. 7, Issue 1
Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures
book, January 1999
- Shah, Jagdeep
- Springer Series in Solid-State Sciences
Grand challenges in basic energy sciences
journal, July 2008
- Fleming, Graham R.; Ratner, Mark A.
- Physics Today, Vol. 61, Issue 7
Analysis of computational EELS modelling results for MgO-based systems
journal, July 2010
- Seabourne, Che R.; Scott, Andrew J.; Vaughan, Gareth
- Ultramicroscopy, Vol. 110, Issue 8
Femtosecond XANES Study of the Light-Induced Spin Crossover Dynamics in an Iron(II) Complex
journal, January 2009
- Bressler, Ch.; Milne, C.; Pham, V. -T.
- Science, Vol. 323, Issue 5913
Femtosecond Electron and Spin Dynamics in Films
journal, June 2003
- Rhie, H. -S.; Dürr, H. A.; Eberhardt, W.
- Physical Review Letters, Vol. 90, Issue 24
Calculating condensed matter properties using the KKR-Green's function method—recent developments and applications
journal, August 2011
- Ebert, H.; Ködderitzsch, D.; Minár, J.
- Reports on Progress in Physics, Vol. 74, Issue 9
Heat transport through interfaces with and without misfit dislocation arrays
journal, October 2012
- Hanisch-Blicharski, Anja; Krenzer, Boris; Wall, Simone
- Journal of Materials Research, Vol. 27, Issue 21
Coherent Atomic Motions in a Nanostructure Studied by Femtosecond X-ray Diffraction
journal, December 2004
- Bargheer, M.; Zhavoronkov, N.; Gritsai, Y.
- Science, Vol. 306, Issue 5702
X‐Ray Characteristic Temperatures of Some II—VI Ionic Compounds
journal, September 1964
- Baldwin, T. O.; Tompson, C. W.
- The Journal of Chemical Physics, Vol. 41, Issue 5
Ultrafast spin-transfer torque driven by femtosecond pulsed-laser excitation
journal, July 2014
- Schellekens, A. J.; Kuiper, K. C.; de Wit, R. R. J. C.
- Nature Communications, Vol. 5, Issue 1
Ultrafast electron diffraction from non-equilibrium phonons in femtosecond laser heated Au films
journal, January 2016
- Chase, T.; Trigo, M.; Reid, A. H.
- Applied Physics Letters, Vol. 108, Issue 4
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Electronic Structure of Warm Dense Copper Studied by Ultrafast X-Ray Absorption Spectroscopy
journal, April 2011
- Cho, B. I.; Engelhorn, K.; Correa, A. A.
- Physical Review Letters, Vol. 106, Issue 16
Review of the Theoretical Description of Time-Resolved Angle-Resolved Photoemission Spectroscopy in Electron-Phonon Mediated Superconductors: Review of the theoretical description of time-resolved angle-resolved photoemission spectroscopy ⋅⋅⋅
journal, July 2017
- Kemper, A. F.; Sentef, M. A.; Moritz, B.
- Annalen der Physik, Vol. 529, Issue 9
Thermal boundary resistance
journal, July 1989
- Swartz, E. T.; Pohl, R. O.
- Reviews of Modern Physics, Vol. 61, Issue 3, p. 605-668
Multiple phonon processes contributing to inelastic scattering during thermal boundary conductance at solid interfaces
journal, July 2009
- Hopkins, Patrick E.
- Journal of Applied Physics, Vol. 106, Issue 1
Thickness-dependent electron–lattice equilibration in laser-excited thin bismuth films
journal, November 2015
- Sokolowski-Tinten, K.; Li, R. K.; Reid, A. H.
- New Journal of Physics, Vol. 17, Issue 11
PHON: A program to calculate phonons using the small displacement method
journal, December 2009
- Alfè, Dario
- Computer Physics Communications, Vol. 180, Issue 12
Femtosecond modification of electron localization and transfer of angular momentum in nickel
journal, August 2007
- Stamm, C.; Kachel, T.; Pontius, N.
- Nature Materials, Vol. 6, Issue 10
Transient electronic and magnetic structures of nickel heated by ultrafast laser pulses
journal, September 2009
- Kachel, T.; Pontius, N.; Stamm, C.
- Physical Review B, Vol. 80, Issue 9
Theory of electronic relaxation in a metal excited by an ultrashort optical pump
journal, March 2014
- Baranov, V. V.; Kabanov, V. V.
- Physical Review B, Vol. 89, Issue 12
P-V-T equation of state of periclase from synchrotron radiation measurements
journal, February 2000
- Dewaele, Agnès; Fiquet, Guillaume; Andrault, Denis
- Journal of Geophysical Research: Solid Earth, Vol. 105, Issue B2
FemtoSpeX: a versatile optical pump–soft X-ray probe facility with 100 fs X-ray pulses of variable polarization
journal, August 2014
- Holldack, Karsten; Bahrdt, Johannes; Balzer, Andreas
- Journal of Synchrotron Radiation, Vol. 21, Issue 5
Theory of out-of-equilibrium ultrafast relaxation dynamics in metals
journal, November 2017
- Maldonado, Pablo; Carva, Karel; Flammer, Martina
- Physical Review B, Vol. 96, Issue 17
Symmetry Breaking Instabilities of an In Vitro Biological System
journal, July 1995
- Sekimoto, Ken; Mori, Naoki; Tawada, Katsuhisa
- Physical Review Letters, Vol. 75, Issue 1
Electronic Kapitza conductance due to inelastic electron-boundary scattering
journal, October 1998
- Sergeev, A. V.
- Physical Review B, Vol. 58, Issue 16
Ultrafast Electron Relaxation in Superconducting by Time-Resolved Photoelectron Spectroscopy
journal, November 2007
- Perfetti, L.; Loukakos, P. A.; Lisowski, M.
- Physical Review Letters, Vol. 99, Issue 19
Mössbauer Spectroscopy and Transition Metal Chemistry: Fundamentals and Applications
book, January 2011
- Gütlich, Philipp; Bill, Eckhard; Trautwein, Alfred X.
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
Nonequilibrium electron and lattice dynamics of strongly correlated Bi 2 Sr 2 CaCu 2 O 8+δ single crystals
journal, April 2018
- Konstantinova, Tatiana; Rameau, Jonathan D.; Reid, Alexander H.
- Science Advances, Vol. 4, Issue 4
Chemical and electronic properties of Fe/MgO/Ge heterostructures for spin electronics
journal, April 2011
- Petti, D.; Cantoni, M.; Rinaldi, C.
- Journal of Physics: Conference Series, Vol. 292
Nanoscale interface confinement of ultrafast spin transfer torque driving non-uniform spin dynamics
journal, April 2017
- Razdolski, Ilya; Alekhin, Alexandr; Ilin, Nikita
- Nature Communications, Vol. 8, Issue 1
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Theory of thermal relaxation of electrons in metals
journal, September 1987
- Allen, Philip B.
- Physical Review Letters, Vol. 59, Issue 13
Influence of laser-excited electron distributions on the X-ray magnetic circular dichroism spectra: Implications for femtosecond demagnetization in Ni
journal, June 2009
- Carva, K.; Legut, D.; Oppeneer, P. M.
- EPL (Europhysics Letters), Vol. 86, Issue 5
Temperature dependence of X-ray absorption and nuclear magnetic resonance spectra: probing quantum vibrations of light elements in oxides
journal, January 2017
- Nemausat, Ruidy; Gervais, Christel; Brouder, Christian
- Physical Chemistry Chemical Physics, Vol. 19, Issue 8
Phonon-induced long-lasting nonequilibrium in the electron system of a laser-excited solid
journal, May 2019
- Weber, S. T.; Rethfeld, B.
- Physical Review B, Vol. 99, Issue 17
Debye- waller factors for alkaline earth oxides
journal, December 1982
- Singh, R. K.; Sanyal, S. P.
- physica status solidi (b), Vol. 114, Issue 2
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
Engineered materials for all-optical helicity-dependent magnetic switching
journal, February 2014
- Mangin, S.; Gottwald, M.; Lambert, C-H.
- Nature Materials, Vol. 13, Issue 3
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
Hot electron lifetimes in metals probed by time-resolved two-photon photoemission
journal, August 2015
- Bauer, M.; Marienfeld, A.; Aeschlimann, M.
- Progress in Surface Science, Vol. 90, Issue 3
Role of dispersion on phononic thermal boundary conductance
journal, October 2010
- Duda, John C.; Beechem, Thomas E.; Smoyer, Justin L.
- Journal of Applied Physics, Vol. 108, Issue 7
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021
- Chen, Ruyi; Cui, Qirui; Liao, Liyang
- Nature Communications, Vol. 12, Issue 1
X-ray absorption study at the Mg and O K edges of ultrathin MgO epilayers on Ag(001)
journal, January 2004
- Luches, P.; D’Addato, S.; Valeri, S.
- Physical Review B, Vol. 69, Issue 4
Electronic structure of magnetic Fe/MgO/Fe/Co multilayer structure by NEXAFS spectroscopy
journal, April 2017
- Singh, Jitendra Pal; Gautam, Sanjeev; Lim, Weon Cheol
- Vacuum, Vol. 138
Mössbauer Spectroscopy and Transition Metal Chemistry
book, January 1978
- Gütlich, Philipp; Link, Rainer; Trautwein, Alfred X.
- Inorganic Chemistry Concepts
Electron and lattice dynamics following optical excitation of metals
journal, January 2000
- Hohlfeld, J.; Wellershoff, S. -S.; Güdde, J.
- Chemical Physics, Vol. 251, Issue 1-3
Improved tetrahedron method for Brillouin-zone integrations
journal, June 1994
- Blöchl, Peter E.; Jepsen, O.; Andersen, O. K.
- Physical Review B, Vol. 49, Issue 23
Controlling the Competition between Optically Induced Ultrafast Spin-Flip Scattering and Spin Transport in Magnetic Multilayers
journal, May 2013
- Turgut, Emrah; La-o-vorakiat, Chan; Shaw, Justin M.
- Physical Review Letters, Vol. 110, Issue 19
Strongly Coupled Optical Phonons in the Ultrafast Dynamics of the Electronic Energy and Current Relaxation in Graphite
journal, October 2005
- Kampfrath, Tobias; Perfetti, Luca; Schapper, Florian
- Physical Review Letters, Vol. 95, Issue 18
Thermal Boundary Resistance.
journal, August 1971
- Budd, H.; Vannimenus, J.
- Physical Review Letters, Vol. 27, Issue 6
Thermal Boundary Resistance
journal, June 1971
- Budd, H.; Vannimenus, J.
- Physical Review Letters, Vol. 26, Issue 26
Influence of laser-excited electron distributions on the x-ray magnetic circular dichroism spectra: Implications for femtosecond demagnetization in Ni
text, January 2009
- Carva, K.; Legut, D.; Oppeneer, P. M.
- arXiv