Ultrafast dynamics of hot charge carriers in an oxide semiconductor probed by femtosecond spectroscopic ellipsometry
(2020) In New Journal of Physics 22(8).- Abstract
Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of Mahan excitons. In this work, we disentangle their dynamics and contributions to the optical response of a ZnO thin film. Using broadband pump-probe ellipsometry, we can directly and unambiguously obtain the real and imaginary part of the transient dielectric function which we compare with first-principles simulations. We find interband and excitonic absorption partially blocked and screened by the photo-excited electron occupation of the conduction band and hole occupation of the valence band... (More)
Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of Mahan excitons. In this work, we disentangle their dynamics and contributions to the optical response of a ZnO thin film. Using broadband pump-probe ellipsometry, we can directly and unambiguously obtain the real and imaginary part of the transient dielectric function which we compare with first-principles simulations. We find interband and excitonic absorption partially blocked and screened by the photo-excited electron occupation of the conduction band and hole occupation of the valence band (absorption bleaching). Exciton absorption turns spectrally narrower upon pumping and sustains the Mott transition, indicating Mahan excitons. Simultaneously, intra-valence-band transitions occur at sub-picosecond time scales after holes scatter to the edge of the Brillouin zone. Our results pave new ways for the understanding of non-equilibrium charge-carrier dynamics in materials by reliably distinguishing between changes in absorption coefficient and refractive index, thereby separating competing processes. This information will help to overcome the limitations of materials for high-power optical devices that owe their properties from dynamics in the ultrafast regime.
(Less)
- author
- publishing date
- 2020-08
- type
- Contribution to journal
- publication status
- published
- keywords
- ellipsometry, exciton-phonon interaction, high excitation, Mahan exciton, transient spectroscopy, ZnO
- in
- New Journal of Physics
- volume
- 22
- issue
- 8
- article number
- 083066
- publisher
- IOP Publishing
- external identifiers
-
- scopus:85090423186
- ISSN
- 1367-2630
- DOI
- 10.1088/1367-2630/aba7f3
- language
- English
- LU publication?
- no
- additional info
- Publisher Copyright: © 2020 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.
- id
- d08810c1-b2a4-4c9d-b555-034be6020e02
- date added to LUP
- 2022-04-19 14:42:27
- date last changed
- 2023-12-18 14:50:06
@article{d08810c1-b2a4-4c9d-b555-034be6020e02,
abstract = {{<p>Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of Mahan excitons. In this work, we disentangle their dynamics and contributions to the optical response of a ZnO thin film. Using broadband pump-probe ellipsometry, we can directly and unambiguously obtain the real and imaginary part of the transient dielectric function which we compare with first-principles simulations. We find interband and excitonic absorption partially blocked and screened by the photo-excited electron occupation of the conduction band and hole occupation of the valence band (absorption bleaching). Exciton absorption turns spectrally narrower upon pumping and sustains the Mott transition, indicating Mahan excitons. Simultaneously, intra-valence-band transitions occur at sub-picosecond time scales after holes scatter to the edge of the Brillouin zone. Our results pave new ways for the understanding of non-equilibrium charge-carrier dynamics in materials by reliably distinguishing between changes in absorption coefficient and refractive index, thereby separating competing processes. This information will help to overcome the limitations of materials for high-power optical devices that owe their properties from dynamics in the ultrafast regime. </p>}},
author = {{Richter, Steffen and Herrfurth, Oliver and Espinoza, Shirly and Rebarz, Mateusz and Kloz, Miroslav and Leveillee, Joshua A. and Schleife, André and Zollner, Stefan and Grundmann, Marius and Andreasson, Jakob and Schmidt-Grund, Rüdiger}},
issn = {{1367-2630}},
keywords = {{ellipsometry; exciton-phonon interaction; high excitation; Mahan exciton; transient spectroscopy; ZnO}},
language = {{eng}},
number = {{8}},
publisher = {{IOP Publishing}},
series = {{New Journal of Physics}},
title = {{Ultrafast dynamics of hot charge carriers in an oxide semiconductor probed by femtosecond spectroscopic ellipsometry}},
url = {{http://dx.doi.org/10.1088/1367-2630/aba7f3}},
doi = {{10.1088/1367-2630/aba7f3}},
volume = {{22}},
year = {{2020}},
}