Hot carrier extraction from 2D semiconductor photoelectrodes
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arXiv
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| Format: | Preprint |
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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 |