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Ultrafast Hot Carrier Injection in Au/GaN: The Role of Band Bending and the Interface Band Structure

Journal Article · · Journal of Physical Chemistry Letters
 [1];  [1]
  1. California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
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Plasmon photochemistry can potentially play a significant role in photocatalysis. To realize this potential, it is critical to enhance the plasmon excited hot carrier transfer and collection. However, the lack of atomistic understanding of the carrier transfer across the interface, especially when the carrier is still "hot", makes it challenging to design a more efficient system. In this work, we apply the nonadiabatic molecular dynamics simulation to study hot carrier dynamics in the system of a Au nanocluster on top of a GaN surface. By setting up the initial excited hole in Au, the carrier transfer from Au to GaN is found to be on a subpicosecond time scale. The hot hole first cools to the band edge of Au d-states while it transfers to GaN. After the hole has cooled down to the band edge of GaN, we find that some of the charges can return back to Au. By applying different external potentials to mimic the Schottky barrier band bending, the returning charge can be reduced, demonstrating the importance of the internal electric field. Finally, with the understanding of the carrier transfer's pathway, we suggest that a ZnO layer between GaN and Au can effectively block the "cold" carrier from returning back to Au but still allow the hot carrier to transfer from Au to GaN.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES), Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-05CH11231; SC0004993
OSTI ID:
1783094
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 20 Vol. 10; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
energy
gold
nanoclusters
nitrides
oxides