Multiple Exciton Generation for Photoelectrochemical Hydrogen Evolution Reactions with Quantum Yields Exceeding 100%

Matthew Beard; Ryan Crisp; John Turner; Gregory Pach; Yong Yan; Boris Chernomordik; Ashley Marshall; Jing Gu

doi:10.1038/nenergy.2017.52

Multiple Exciton Generation for Photoelectrochemical Hydrogen Evolution Reactions with Quantum Yields Exceeding 100%

Matthew Beard, Ryan Crisp, John Turner, Gregory Pach, Yong Yan, Boris Chernomordik, Ashley Marshall, Jing Gu

Chemistry and Nanoscience

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	American English
Article number	Article No. 17052
Number of pages	7
Journal	Nature Energy
Volume	2
Issue number	5
DOIs	https://doi.org/10.1038/nenergy.2017.52 https://doi.org/10.1038/nenergy.2017.52
State	Published - 27 Mar 2017

Bibliographical note

Publisher Copyright:
© 2017 Macmillan Publishers Limited, part of Springer Nature.

NREL Publication Number

NREL/JA-5900-66234

Keywords

multiple exciton generation
QD
quantum dots
solar energy conversion
solar fuels
solar-photochemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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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 - Beard, Matthew

AU - Crisp, Ryan

AU - Turner, John

AU - Pach, Gregory

AU - Yan, Yong

AU - Chernomordik, Boris

AU - Marshall, Ashley

AU - Gu, Jing

PY - 2017/3/27

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N2 - 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.

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.

KW - multiple exciton generation

KW - QD

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KW - solar energy conversion

KW - solar fuels

KW - solar-photochemistry

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JO - Nature Energy

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Multiple Exciton Generation for Photoelectrochemical Hydrogen Evolution Reactions with Quantum Yields Exceeding 100%

Abstract

Bibliographical note

NREL Publication Number

Keywords

UN SDGs

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