Hot carrier extraction from 2D semiconductor photoelectrodes

Fuente: arXiv
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Hauptverfasser: Austin, Rachelle, Farah, Yusef, Sayer, Thomas, Luther, Brad M., Montoya-Castillo, Andrés, Krummel, Amber, Sambur, Justin
Format: Preprint
Veröffentlicht: 2022
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author Austin, Rachelle
Farah, Yusef
Sayer, Thomas
Luther, Brad M.
Montoya-Castillo, Andrés
Krummel, Amber
Sambur, Justin
author_facet Austin, Rachelle
Farah, Yusef
Sayer, Thomas
Luther, Brad M.
Montoya-Castillo, Andrés
Krummel, Amber
Sambur, Justin
contents Hot carrier-based energy conversion systems could double the efficiency of conventional solar energy technology or drive photochemical reactions that would not be possible using fully thermalized, ``cool'' carriers, but current strategies require expensive multi-junction architectures. Using an unprecedented combination of photoelectrochemical and in situ transient absorption spectroscopy measurements, we demonstrate ultrafast (<50 fs) hot exciton and free carrier extraction under applied bias in a proof-of-concept photoelectrochemical solar cell made from earth-abundant and potentially inexpensive monolayer (ML) MoS2. Our approach facilitates ultrathin 7Åcharge transport distances over 1 cm^2 areas by intimately coupling ML-MoS2 to an electron-selective solid contact and a hole-selective electrolyte contact. Our theoretical investigations of the spatial distribution of exciton states suggest greater electronic coupling between hot exciton states located on peripheral S atoms and neighboring contacts likely facilitates ultrafast charge transfer. Our work delineates future 2D semiconductor design strategies for practical implementation in ultrathin photovoltaic and solar fuels applications.
format Preprint
id arxiv_https___arxiv_org_abs_2210_13588
institution arXiv
publishDate 2022
record_format arxiv
spellingShingle Hot carrier extraction from 2D semiconductor photoelectrodes
Austin, Rachelle
Farah, Yusef
Sayer, Thomas
Luther, Brad M.
Montoya-Castillo, Andrés
Krummel, Amber
Sambur, Justin
Materials Science
Mesoscale and Nanoscale Physics
Chemical Physics
Hot carrier-based energy conversion systems could double the efficiency of conventional solar energy technology or drive photochemical reactions that would not be possible using fully thermalized, ``cool'' carriers, but current strategies require expensive multi-junction architectures. Using an unprecedented combination of photoelectrochemical and in situ transient absorption spectroscopy measurements, we demonstrate ultrafast (<50 fs) hot exciton and free carrier extraction under applied bias in a proof-of-concept photoelectrochemical solar cell made from earth-abundant and potentially inexpensive monolayer (ML) MoS2. Our approach facilitates ultrathin 7Åcharge transport distances over 1 cm^2 areas by intimately coupling ML-MoS2 to an electron-selective solid contact and a hole-selective electrolyte contact. Our theoretical investigations of the spatial distribution of exciton states suggest greater electronic coupling between hot exciton states located on peripheral S atoms and neighboring contacts likely facilitates ultrafast charge transfer. Our work delineates future 2D semiconductor design strategies for practical implementation in ultrathin photovoltaic and solar fuels applications.
title Hot carrier extraction from 2D semiconductor photoelectrodes
topic Materials Science
Mesoscale and Nanoscale Physics
Chemical Physics
url https://arxiv.org/abs/2210.13588