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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.
Authors:
 [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):
BNL-108525-2015-JA
Journal ID: ISSN 1614-6832; R&D Project: 16060/16060; KC0403020
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 115; Journal Issue: 19; Journal ID: ISSN 1614-6832
Publisher:
Wiley
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
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; cuprous oxide; photoelectrochemistry; solar energy conversion; surface plasmon resonance; Center for Functional Nanomaterials
OSTI Identifier:
1224787

DuChene, Joseph S., Williams, Benjamin P., Johnston-Peck, Aaron C., Qiu, Jingjing, Gomes, Mathieu, Amilhau, Maxime, Bejleri, Donald, Weng, Jiena, Su, Dong, Huo, Fengwei, Stach, Eric A., and Wei, Wei David. Elucidating the sole contribution from electromagnetic near-fields in plasmon-enhanced Cu2O photocathodes. United States: N. p., Web. doi:10.1002/aenm.201501250.
DuChene, Joseph S., Williams, Benjamin P., Johnston-Peck, Aaron C., Qiu, Jingjing, Gomes, Mathieu, Amilhau, Maxime, Bejleri, Donald, Weng, Jiena, Su, Dong, Huo, Fengwei, Stach, Eric A., & Wei, Wei David. Elucidating the sole contribution from electromagnetic near-fields in plasmon-enhanced Cu2O photocathodes. United States. doi:10.1002/aenm.201501250.
DuChene, Joseph S., Williams, Benjamin P., Johnston-Peck, Aaron C., Qiu, Jingjing, Gomes, Mathieu, Amilhau, Maxime, Bejleri, Donald, Weng, Jiena, Su, Dong, Huo, Fengwei, Stach, Eric A., and Wei, Wei David. 2015. "Elucidating the sole contribution from electromagnetic near-fields in plasmon-enhanced Cu2O photocathodes". United States. doi:10.1002/aenm.201501250. https://www.osti.gov/servlets/purl/1224787.
@article{osti_1224787,
title = {Elucidating the sole contribution from electromagnetic near-fields in plasmon-enhanced Cu2O photocathodes},
author = {DuChene, Joseph S. and Williams, Benjamin P. and Johnston-Peck, Aaron C. and Qiu, Jingjing and Gomes, Mathieu and Amilhau, Maxime and Bejleri, Donald and Weng, Jiena and Su, Dong and Huo, Fengwei and Stach, Eric A. and Wei, Wei David},
abstractNote = {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@SiO2 (core@shell) nanoparticles embedded within a Cu2O 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 SiO2 shell thickness (5—22 nm) to systematically tailor the distance between the plasmonic Au nanoparticles and the Cu2O nanowires. A three-fold increase in device photocurrent is achieved upon integrating the Au@SiO2 nanoparticles into the Cu2O 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.},
doi = {10.1002/aenm.201501250},
journal = {Advanced Energy Materials},
number = 19,
volume = 115,
place = {United States},
year = {2015},
month = {11}
}