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. (2020) Ultrafast hot-hole injection modifies hot-electron dynamics in Au/p-GaN heterostructures. Nature Materials, 19 (12). pp. 1312-1318. ISSN 1476-1122. doi:10.1038/s41563-020-0737-1. https://resolver.caltech.edu/CaltechAUTHORS:20181112-073640797
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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.
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| Alternate Title: | Ultrafast Hot-Hole Injection Modifies Hot-Electron Dynamics in Au/p-GaN Heterostructures, Ultrafast Studies of Hot-Hole Dynamics in Au/p-GaN Heterostructures | ||||||||||||||||||
| Additional Information: | © 2020 The Author(s), under exclusive licence to Springer Nature Limited. Received 06 December 2018; Accepted 16 June 2020; Published 27 July 2020. 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. 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. Data availability: The datasets generated and analysed during the study are available from the corresponding authors upon request. Author Contributions: These authors contributed equally: Giulia Tagliabue, Joseph S. DuChene, Mohamed Abdellah. J.S.D., G.T. and H.A.A. conceived the idea, designed the experiments, analysed data and wrote the manuscript with contributions from all authors. M.A., Y.H. and J.S. performed infrared transient absorption spectroscopy experiments. M.A., K.Z., S.E.C. and D.J.G. performed visible transient absorption spectroscopy experiments. A.H. and R.S. performed ab initio theory calculations. J.S.D. and G.T. fabricated and characterized materials. W.-H.C. acquired absorption spectra of materials. H.A.A. supervised the project. All authors have given approval to the final version of the manuscript. The authors declare no competing interests. | ||||||||||||||||||
| Group: | JCAP | ||||||||||||||||||
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| Subject Keywords: | Nanophotonics and plasmonics; Optoelectronic devices and components | ||||||||||||||||||
| Issue or Number: | 12 | ||||||||||||||||||
| DOI: | 10.1038/s41563-020-0737-1 | ||||||||||||||||||
| Record Number: | CaltechAUTHORS:20181112-073640797 | ||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20181112-073640797 | ||||||||||||||||||
| Official Citation: | Tagliabue, G., DuChene, J.S., Abdellah, M. et al. Ultrafast hot-hole injection modifies hot-electron dynamics in Au/p-GaN heterostructures. Nat. Mater. 19, 1312–1318 (2020). https://doi.org/10.1038/s41563-020-0737-1 | ||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||
| ID Code: | 90823 | ||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||
| Deposited By: | Tony Diaz | ||||||||||||||||||
| Deposited On: | 13 Nov 2018 17:36 | ||||||||||||||||||
| Last Modified: | 16 Nov 2021 03:35 |
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