@article{d3304ff6cd434974a00919c2297e4992,
title = "Ultrafast hot-hole injection modifies hot-electron dynamics in Au/p-GaN heterostructures",
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 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.",
author = "Giulia Tagliabue and DuChene, {Joseph S.} and Mohamed Abdellah and Adela Habib and Gosztola, {David J.} and Yocefu Hattori and Cheng, {Wen Hui} and Kaibo Zheng and Canton, {Sophie E.} and Ravishankar Sundararaman and Jacinto S{\'a} and Atwater, {Harry A.}",
note = "Funding Information: This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under award no. DE-SC0004993. A portion of the ultrafast spectroscopy work was performed at the Center for Nanoscale Materials, a US Department of Energy Office of Science User Facility, and supported by the US Department of Energy, Office of Science, under contract no. DE-AC02-06CH11357. G.T. Funding Information: acknowledges support from the Swiss National Science Foundation through the Early Postdoc.Mobility Fellowship, grant no. P2EZP2_159101 and the Advanced Mobility Fellowship, grant no. P300P2_171417. We also thank M. V. Pavliuk for assistance in conducting ultrafast transient absorption spectroscopy measurements from planar Au films on p-GaN substrates. Publisher Copyright: {\textcopyright} 2020, The Author(s), under exclusive licence to Springer Nature Limited.",
year = "2020",
month = dec,
doi = "10.1038/s41563-020-0737-1",
language = "English",
volume = "19",
pages = "1312--1318",
journal = "Nature Materials",
issn = "1476-1122",
publisher = "Nature Publishing Group",
number = "12",
}