Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy
Abstract
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. Finally, 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 populationmore »
- Authors:
-
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Swiss National Science Foundation (SNSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; Humboldt Foundation; Army Research Office (ARO); US Air Force Office of Scientific Research (AFOSR); Defense Advanced Research Projects Agency (DARPA)
- OSTI Identifier:
- 1506355
- Alternate Identifier(s):
- OSTI ID: 1469433
- Grant/Contract Number:
- AC02-05CH11231; W31P4Q-13-1-0017
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Structural Dynamics
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 5; Journal ID: ISSN 2329-7778
- Publisher:
- American Crystallographic Association/AIP
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Cushing, Scott K., Zürch, Michael, Kraus, Peter M., Carneiro, Lucas M., Lee, Angela, Chang, Hung-Tzu, Kaplan, Christopher J., and Leone, Stephen R. Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy. United States: N. p., 2018.
Web. doi:10.1063/1.5038015.
Cushing, Scott K., Zürch, Michael, Kraus, Peter M., Carneiro, Lucas M., Lee, Angela, Chang, Hung-Tzu, Kaplan, Christopher J., & Leone, Stephen R. Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy. United States. https://doi.org/10.1063/1.5038015
Cushing, Scott K., Zürch, Michael, Kraus, Peter M., Carneiro, Lucas M., Lee, Angela, Chang, Hung-Tzu, Kaplan, Christopher J., and Leone, Stephen R. Tue .
"Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy". United States. https://doi.org/10.1063/1.5038015. https://www.osti.gov/servlets/purl/1506355.
@article{osti_1506355,
title = {Hot phonon and carrier relaxation in Si(100) determined by transient extreme ultraviolet spectroscopy},
author = {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.},
abstractNote = {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. Finally, 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.},
doi = {10.1063/1.5038015},
journal = {Structural Dynamics},
number = 5,
volume = 5,
place = {United States},
year = {Tue Sep 11 00:00:00 EDT 2018},
month = {Tue Sep 11 00:00:00 EDT 2018}
}
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Figures / Tables:
FIG. 1.: Critical points and core-hole modification of the spectrum of the Si 2p L23 edge. (a) Band structure of silicon along the L-C-X path, highlighting the $\Delta$1, L1, and L3 critical points. The k-space directions are marked. Note L is at $^1_2, ^1_ 2 ,^1_ 2$ and $\Delta$ ismore »
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Works referencing / citing this record:
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