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Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy

Cushing, Scott K. and Zürch, Michael and Kraus, Peter M. and Carneiro, Lucas M. and Lee, Angela and Chang, Hung-Tzu and Kaplan, Christopher J. and Leone, Stephen R. (2018) Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy. Structural Dynamics, 5 (5). Art. No. 054302. ISSN 2329-7778. doi:10.1063/1.5038015.

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The thermalization of hot carriers and phonons gives direct insight into the scattering processes that mediate electrical and thermal transport. Obtaining the scattering rates for both hot carriers and phonons currently requires multiple measurements with incommensurate timescales. Here, transient extreme-ultraviolet (XUV) spectroscopy on the silicon 2p core level at 100 eV is used to measure hot carrier and phonon thermalization in Si(100) from tens of femtoseconds to 200 ps, following photoexcitation of the indirect transition to the Δ valley at 800 nm. The ground state XUV spectrum is first theoretically predicted using a combination of a single plasmon pole model and the Bethe-Salpeter equation with density functional theory. The excited state spectrum is predicted by incorporating the electronic effects of photo-induced state-filling, broadening, and band-gap renormalization into the ground state XUV spectrum. A time-dependent lattice deformation and expansion is also required to describe the excited state spectrum. The kinetics of these structural components match the kinetics of phonons excited from the electron-phonon and phonon-phonon scattering processes following photoexcitation. Separating the contributions of electronic and structural effects on the transient XUV spectra allows the carrier population, the population of phonons involved in inter- and intra-valley electron-phonon scattering, and the population of phonons involved in phonon-phonon scattering to be quantified as a function of delay time.

Item Type:Article
Related URLs:
URLURL TypeDescription Paper
Cushing, Scott K.0000-0003-3538-2259
Lee, Angela0000-0001-5388-8400
Chang, Hung-Tzu0000-0001-7378-8212
Kaplan, Christopher J.0000-0002-5873-9487
Leone, Stephen R.0000-0003-1819-1338
Alternate Title:Valley-Specific Hot Phonon and Carrier Relaxation Pathways in Si(100) Determined by Transient Extreme Ultraviolet Spectroscopy
Additional Information:© 2018 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license ( Received 30 April 2018; accepted 22 August 2018; published online 11 September 2018. This work was supported by the Physical Chemistry of Inorganic Nanostructures Program, KC3103, Office of Basic Energy Sciences of the United States Department of Energy under Contract No. DE-AC02-05CH11231 through Materials Science and Engineering. S.K.C. acknowledges the support from the Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Solar Energy Technologies Office. P.M.K. acknowledges the support from the Swiss National Science Foundation (P2EZP2_165252). M.Z. acknowledges the support from the Humboldt Foundation. M.Z. also acknowleges the support of the Army Research Office (ARO) (WN911NF-14-1-0383). C.J.K. was supported by Defense Advanced Research Projects Agency PULSE program through Grant No. W31P4Q-13-1-0017. H.-T. C. acknowledges support by the Air Force Office of Scientific Research (AFOSR) (FA9550-15-1-0037).
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-05CH11231
Swiss National Science Foundation (SNSF)P2EZP2_165252
Alexander von Humboldt FoundationUNSPECIFIED
Army Research Office (ARO)WN911NF-14-1-0383
Defense Advanced Research Projects Agency (DARPA)W31P4Q-13-1-0017
Air Force Office of Scientific Research (AFOSR)FA9550-15-1-0037
Issue or Number:5
Record Number:CaltechAUTHORS:20180627-095202493
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:87381
Deposited By: George Porter
Deposited On:27 Jun 2018 17:26
Last Modified:15 Nov 2021 20:47

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