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Ultrafast hot-hole injection modifies hot-electron dynamics in Au/p-GaN heterostructures

Tagliabue, Giulia ; DuChene, Joseph S. ; Abdellah, Mohamed LU ; Habib, Adela ; Gosztola, David J. ; Hattori, Yocefu ; Cheng, Wen Hui ; Zheng, Kaibo LU ; Canton, Sophie E. LU and Sundararaman, Ravishankar , et al. (2020) In Nature Materials 19(12). p.1312-1318
Abstract

A fundamental understanding of hot-carrier dynamics in photo-excited metal nanostructures is needed to unlock their potential for photodetection and photocatalysis. Despite numerous studies on the ultrafast dynamics of hot electrons, so far, the temporal evolution of hot holes in metal–semiconductor heterostructures remains unknown. Here, we report ultrafast (t < 200 fs) hot-hole injection from Au nanoparticles into the valence band of p-type GaN. The removal of hot holes from below the Au Fermi level is observed to substantially alter the thermalization dynamics of hot electrons, reducing the peak electronic temperature and the electron–phonon coupling time of the Au nanoparticles. First-principles calculations reveal that hot-hole... (More)

A fundamental understanding of hot-carrier dynamics in photo-excited metal nanostructures is needed to unlock their potential for photodetection and photocatalysis. Despite numerous studies on the ultrafast dynamics of hot electrons, so far, the temporal evolution of hot holes in metal–semiconductor heterostructures remains unknown. Here, we report ultrafast (t < 200 fs) hot-hole injection from Au nanoparticles into the valence band of p-type GaN. The removal of hot holes from below the Au Fermi level is observed to substantially alter the thermalization dynamics of hot electrons, reducing the peak electronic temperature and the electron–phonon coupling time of the Au nanoparticles. First-principles calculations reveal that hot-hole injection modifies the relaxation dynamics of hot electrons in Au nanoparticles by modulating the electronic structure of the metal on timescales commensurate with electron–electron scattering. These results advance our understanding of hot-hole dynamics in metal–semiconductor heterostructures and offer additional strategies for manipulating the dynamics of hot carriers on ultrafast timescales.

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Contribution to journal
publication status
published
subject
in
Nature Materials
volume
19
issue
12
pages
7 pages
publisher
Nature Publishing Group
external identifiers
  • pmid:32719510
  • scopus:85088585583
ISSN
1476-1122
DOI
10.1038/s41563-020-0737-1
language
English
LU publication?
yes
id
3c700c11-c0dd-4762-9e42-bf2269a889e0
date added to LUP
2020-08-06 12:38:28
date last changed
2024-04-17 14:00:33
@article{3c700c11-c0dd-4762-9e42-bf2269a889e0,
  abstract     = {{<p>A fundamental understanding of hot-carrier dynamics in photo-excited metal nanostructures is needed to unlock their potential for photodetection and photocatalysis. Despite numerous studies on the ultrafast dynamics of hot electrons, so far, the temporal evolution of hot holes in metal–semiconductor heterostructures remains unknown. Here, we report ultrafast (t &lt; 200 fs) hot-hole injection from Au nanoparticles into the valence band of p-type GaN. The removal of hot holes from below the Au Fermi level is observed to substantially alter the thermalization dynamics of hot electrons, reducing the peak electronic temperature and the electron–phonon coupling time of the Au nanoparticles. First-principles calculations reveal that hot-hole injection modifies the relaxation dynamics of hot electrons in Au nanoparticles by modulating the electronic structure of the metal on timescales commensurate with electron–electron scattering. These results advance our understanding of hot-hole dynamics in metal–semiconductor heterostructures and offer additional strategies for manipulating the dynamics of hot carriers on ultrafast timescales.</p>}},
  author       = {{Tagliabue, Giulia and DuChene, Joseph S. and Abdellah, Mohamed and Habib, Adela and Gosztola, David J. and Hattori, Yocefu and Cheng, Wen Hui and Zheng, Kaibo and Canton, Sophie E. and Sundararaman, Ravishankar and Sá, Jacinto and Atwater, Harry A.}},
  issn         = {{1476-1122}},
  language     = {{eng}},
  number       = {{12}},
  pages        = {{1312--1318}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Materials}},
  title        = {{Ultrafast hot-hole injection modifies hot-electron dynamics in Au/p-GaN heterostructures}},
  url          = {{http://dx.doi.org/10.1038/s41563-020-0737-1}},
  doi          = {{10.1038/s41563-020-0737-1}},
  volume       = {{19}},
  year         = {{2020}},
}