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Ultrafast Studies of Hot-Hole Dynamics in Au/p-GaN Heterostructures

Tagliabue, Giulia and DuChene, Joseph S. and Abdellah, Mohamed and Habib, Adela and Hattori, Yocefu and Zheng, Kaibo and Canton, Sophie E. and Gosztola, David J. and Cheng, Wen-Hui and Sundararaman, Ravishankar and Sá, Jacinto and Atwater, Harry A. (2018) Ultrafast Studies of Hot-Hole Dynamics in Au/p-GaN Heterostructures. . (Submitted)

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Harvesting non-equilibrium hot carriers from photo-excited metal nanoparticles has enabled plasmon-driven photochemical transformations and tunable photodetection with resonant nanoantennas. Despite numerous studies on the ultrafast dynamics of hot electrons, to date, the temporal evolution of hot holes in metal-semiconductor heterostructures remains unknown. An improved understanding of the carrier dynamics in hot-hole-driven systems is needed to help expand the scope of hot-carrier optoelectronics beyond hot-electron-based devices. Here, using ultrafast transient absorption spectroscopy, we show that plasmon-induced hot-hole injection from gold (Au) nanoparticles into the valence band of p-type gallium nitride (p-GaN) occurs within 200 fs, placing hot-hole transfer on a similar timescale as hot-electron transfer. We further observed that the removal of hot holes from below the Au Fermi level exerts a discernible influence on the thermalization of hot electrons above it, reducing the peak electronic temperature and decreasing the electron-phonon coupling time relative to Au samples without a pathway for hot-hole collection. First principles calculations corroborate these experimental observations, suggesting that hot-hole injection modifies the relaxation dynamics of hot electrons in Au nanoparticles through ultrafast modulation of the d-band electronic structure. Taken together, these ultrafast studies substantially advance our understanding of the temporal evolution of hot holes in metal-semiconductor heterostructures and suggest new strategies for manipulating and controlling the energy distributions of hot carriers on ultrafast timescales.

Item Type:Report or Paper (Discussion Paper)
Related URLs:
URLURL TypeDescription Paper
Tagliabue, Giulia0000-0003-4587-728X
DuChene, Joseph S.0000-0002-7145-323X
Cheng, Wen-Hui0000-0003-3233-4606
Sundararaman, Ravishankar0000-0002-0625-4592
Atwater, Harry A.0000-0001-9435-0201
Additional 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 U.S. Department of Energy under Award No. DE-SC0004993. A portion of the ultrafast spectroscopy work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. 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 n. P2EZP2_159101 and the Advanced Mobility Fellowship, grant n. P300P2_171417. Author Contributions: J.S.D., G.T., and H.A.A. conceived the idea, designed the experiments, and wrote the manuscript with contributions from all authors. M.Q., Y.H., and J.S. performed infrared transient absorption spectroscopy experiments. M.Q., K.Z., S.E.C., and D.J.G. performed visible transient absorption spectroscopy experiments. A.H. and R.S. performed theoretical 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.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-06CH11357
Swiss National Science Foundation (SNSF)P2EZP2_159101
Swiss National Science Foundation (SNSF)P300P2_171417
Record Number:CaltechAUTHORS:20181112-073640797
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:90823
Deposited By: Tony Diaz
Deposited On:13 Nov 2018 17:36
Last Modified:27 Nov 2019 00:31

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