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Title: Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%

Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron-hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na 2S solution with a peak external quantum efficiency exceeding 100%. QD photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Finally, our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [5] ; ORCiD logo [4] ;  [4]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); New Jersey Institute of Technology, Newark, NJ (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); San Diego State Univ., San Diego, CA (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5900-66234
Journal ID: ISSN 2058-7546
Grant/Contract Number:
AC36-08GO28308
Type:
Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 2; Journal Issue: 5; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; solar fuels; multiple exciton generation; quantum dots; QD; solar energy conversion; hydrogen energy; photocatalysis; photochemistry
OSTI Identifier:
1351583

Yan, Yong, Crisp, Ryan W., Gu, Jing, Chernomordik, Boris D., Pach, Gregory F., Marshall, Ashley R., Turner, John A., and Beard, Matthew C.. Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%. United States: N. p., Web. doi:10.1038/nenergy.2017.52.
Yan, Yong, Crisp, Ryan W., Gu, Jing, Chernomordik, Boris D., Pach, Gregory F., Marshall, Ashley R., Turner, John A., & Beard, Matthew C.. Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%. United States. doi:10.1038/nenergy.2017.52.
Yan, Yong, Crisp, Ryan W., Gu, Jing, Chernomordik, Boris D., Pach, Gregory F., Marshall, Ashley R., Turner, John A., and Beard, Matthew C.. 2017. "Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%". United States. doi:10.1038/nenergy.2017.52. https://www.osti.gov/servlets/purl/1351583.
@article{osti_1351583,
title = {Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%},
author = {Yan, Yong and Crisp, Ryan W. and Gu, Jing and Chernomordik, Boris D. and Pach, Gregory F. and Marshall, Ashley R. and Turner, John A. and Beard, Matthew C.},
abstractNote = {Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron-hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na2S solution with a peak external quantum efficiency exceeding 100%. QD photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Finally, our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.},
doi = {10.1038/nenergy.2017.52},
journal = {Nature Energy},
number = 5,
volume = 2,
place = {United States},
year = {2017},
month = {4}
}

Works referenced in this record:

Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
journal, March 1961
  • Shockley, William; Queisser, Hans J.
  • Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519
  • DOI: 10.1063/1.1736034