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Title: Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel

Abstract

Femtosecond laser excitation of solid-state systems creates out-of-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering, we gain a detailed understanding of the complex nonequilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wave-vector-resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy, a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond time scale. We determine the evolving nonequilibrium phonon occupations, which we find to deviate markedly from thermal occupations.

Authors:
ORCiD logo; ; ; ; ; ; ; ORCiD logo; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1604496
Alternate Identifier(s):
OSTI ID: 1608315
Grant/Contract Number:  
AC02-05-CH11231; AC02-76SF00515; 2015.0060; 737709; 15–08740Y; 278162697-SFB 1242
Resource Type:
Published Article
Journal Name:
Physical Review B
Additional Journal Information:
Journal Name: Physical Review B Journal Volume: 101 Journal Issue: 10; 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; Lattice dynamics; Magneto-optical spectra; Ferromagnets; Density functional calculations; Electron diffraction; Femtosecond laser irradiation; First-principles calculations; Photoexcitation

Citation Formats

Maldonado, P., Chase, T., Reid, A. H., Shen, X., Li, R. K., Carva, K., Payer, T., Horn von Hoegen, M., Sokolowski-Tinten, K., Wang, X. J., Oppeneer, P. M., and Dürr, H. A. Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel. United States: N. p., 2020. Web. doi:10.1103/PhysRevB.101.100302.
Maldonado, P., Chase, T., Reid, A. H., Shen, X., Li, R. K., Carva, K., Payer, T., Horn von Hoegen, M., Sokolowski-Tinten, K., Wang, X. J., Oppeneer, P. M., & Dürr, H. A. Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel. United States. doi:https://doi.org/10.1103/PhysRevB.101.100302
Maldonado, P., Chase, T., Reid, A. H., Shen, X., Li, R. K., Carva, K., Payer, T., Horn von Hoegen, M., Sokolowski-Tinten, K., Wang, X. J., Oppeneer, P. M., and Dürr, H. A. Thu . "Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel". United States. doi:https://doi.org/10.1103/PhysRevB.101.100302.
@article{osti_1604496,
title = {Tracking the ultrafast nonequilibrium energy flow between electronic and lattice degrees of freedom in crystalline nickel},
author = {Maldonado, P. and Chase, T. and Reid, A. H. and Shen, X. and Li, R. K. and Carva, K. and Payer, T. and Horn von Hoegen, M. and Sokolowski-Tinten, K. and Wang, X. J. and Oppeneer, P. M. and Dürr, H. A.},
abstractNote = {Femtosecond laser excitation of solid-state systems creates out-of-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering, we gain a detailed understanding of the complex nonequilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wave-vector-resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy, a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond time scale. We determine the evolving nonequilibrium phonon occupations, which we find to deviate markedly from thermal occupations.},
doi = {10.1103/PhysRevB.101.100302},
journal = {Physical Review B},
number = 10,
volume = 101,
place = {United States},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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DOI: https://doi.org/10.1103/PhysRevB.101.100302

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