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

Yong Yan; Ryan W. Crisp; Jing Gu; Boris D. Chernomordik; Gregory F. Pach; Ashley R. Marshall; John A. Turner; Matthew C. Beard

doi:10.1038/nenergy.2017.52

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

Yong Yan, Ryan W. Crisp, Jing Gu, Boris D. Chernomordik, Gregory F. Pach, Ashley R. Marshall, John A. Turner, Matthew C. Beard

Chemistry and Environmental Science

Research output: Contribution to journal › Article › peer-review

176 Scopus citations

Abstract

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 2 S 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. Our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.

Original language	English (US)
Article number	17052
Journal	Nature Energy
Volume	2
Issue number	5
DOIs	https://doi.org/10.1038/nenergy.2017.52
State	Published - Mar 27 2017

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology

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10.1038/nenergy.2017.52

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title = "Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%",

abstract = "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 2 S 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. Our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.",

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AU - Yan, Yong

AU - Crisp, Ryan W.

AU - Gu, Jing

AU - Chernomordik, Boris D.

AU - Pach, Gregory F.

AU - Marshall, Ashley R.

AU - Turner, John A.

AU - Beard, Matthew C.

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AB - 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 2 S 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. Our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.

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

Abstract

All Science Journal Classification (ASJC) codes

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