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Title: Elucidating the sole contribution from electromagnetic near-fields in plasmon-enhanced Cu 2O photocathodes

Despite many promising reports of plasmon-enhanced photocatalysis, the inability to identify the individual contributions from multiple enhancement mechanisms has delayed the development of general design rules for engineering efficient plasmonic photocatalysts. Herein, we construct a plasmonic photocathode comprised of Au@SiO 2 (core@shell) nanoparticles embedded within a Cu 2O nanowire network to exclusively examine the contribution from one such mechanism: electromagnetic near-field enhancement. The influence of the local electromagnetic field intensity is correlated with the overall light-harvesting efficiency of the device through variation of the SiO 2 shell thickness (5—22 nm) to systematically tailor the distance between the plasmonic Au nanoparticles and the Cu 2O nanowires. A three-fold increase in device photocurrent is achieved upon integrating the Au@SiO 2 nanoparticles into the Cu 2O nanowire network, further enabling a ~40% reduction in semiconductor film thickness while maintaining photocathode performance. Photoelectrochemical results are further correlated with photoluminescence studies and optical simulations to confirm that the near-field enhancement is the sole mechanism responsible for increased light absorption in the plasmonic photocathode.
 [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [3] ;  [2] ;  [3] ;  [2] ;  [1]
  1. Univ. of Florida, Gainesville, FL (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Nanjing Tech Univ., Nanjing (China)
Publication Date:
Report Number(s):
Journal ID: ISSN 1614-6832; R&D Project: 16060/16060; KC0403020
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 115; Journal Issue: 19; Journal ID: ISSN 1614-6832
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
77 NANOSCIENCE AND NANOTECHNOLOGY; cuprous oxide; photoelectrochemistry; solar energy conversion; surface plasmon resonance; Center for Functional Nanomaterials
OSTI Identifier: