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Title: 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 L 3 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 L 3 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];  [1];  [1];  [2];  [1];  [1];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Univ. of Duisburg-Essen (Germany). Center for Nanointegration Duisburg-Essen (CENIDE)
  2. Forschungszentrum Jülich (Germany). Peter-Grünberg-Inst.
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
German Research Foundation (DFG); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). 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. 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., and Eschenlohr, A. Tue . "Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure". United States. doi:10.1103/PhysRevB.100.174301.
@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 = {2019},
month = {11}
}

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