Non-Equilibrium Pathways for Excitation of Bulk and Surface Phonons through Anharmonic Coupling

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Hauptverfasser: Brand, C., Tinnemann, V., Hanisch-Blicharski, A., Tajik, M., Fortmann, J. D., Kaßen, A., Thiemann, F., Hoegen, M. Horn-von
Format: Preprint
Veröffentlicht: 2023
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author Brand, C.
Tinnemann, V.
Hanisch-Blicharski, A.
Tajik, M.
Fortmann, J. D.
Kaßen, A.
Thiemann, F.
Hoegen, M. Horn-von
author_facet Brand, C.
Tinnemann, V.
Hanisch-Blicharski, A.
Tajik, M.
Fortmann, J. D.
Kaßen, A.
Thiemann, F.
Hoegen, M. Horn-von
contents Upon impulsive optical excitation of solid-state materials, the non-equilibrium flow of energy from the excited electronic system to the lattice degrees of freedom typically happens in a few picoseconds. Here we identified the surface of thin Bi films grown on Si(001) as an additional subsystem which is excited much slower on a 100 ps timescale that is caused by decoupling due to mismatched phonon dispersions relations of bulk and surface. Anharmonic coupling among the phonon systems provides pathways for excitations which exhibits a 1/T-dependence causing a speed-up of surface excitation at higher temperatures. A quantitative justification is provided by phonon Umklapp processes from lattice thermal conductivity of the Bi bulk. Three-temperature model simulations reveal a pronounced non-equilibrium situation up to nanoseconds: initially, the surface is colder than the bulk, that situation is then inverted during cooling and the surface feeds energy back into the bulk phonon system.
format Preprint
id arxiv_https___arxiv_org_abs_2310_15740
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Non-Equilibrium Pathways for Excitation of Bulk and Surface Phonons through Anharmonic Coupling
Brand, C.
Tinnemann, V.
Hanisch-Blicharski, A.
Tajik, M.
Fortmann, J. D.
Kaßen, A.
Thiemann, F.
Hoegen, M. Horn-von
Mesoscale and Nanoscale Physics
Upon impulsive optical excitation of solid-state materials, the non-equilibrium flow of energy from the excited electronic system to the lattice degrees of freedom typically happens in a few picoseconds. Here we identified the surface of thin Bi films grown on Si(001) as an additional subsystem which is excited much slower on a 100 ps timescale that is caused by decoupling due to mismatched phonon dispersions relations of bulk and surface. Anharmonic coupling among the phonon systems provides pathways for excitations which exhibits a 1/T-dependence causing a speed-up of surface excitation at higher temperatures. A quantitative justification is provided by phonon Umklapp processes from lattice thermal conductivity of the Bi bulk. Three-temperature model simulations reveal a pronounced non-equilibrium situation up to nanoseconds: initially, the surface is colder than the bulk, that situation is then inverted during cooling and the surface feeds energy back into the bulk phonon system.
title Non-Equilibrium Pathways for Excitation of Bulk and Surface Phonons through Anharmonic Coupling
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2310.15740