Femtosecond time-resolved two-photon photoemission studies of ultrafast carrier relaxation in Cu2O photoelectrodes
Abstract
Abstract Cuprous oxide (Cu 2 O) is a promising material for solar-driven water splitting to produce hydrogen. However, the relatively small accessible photovoltage limits the development of efficient Cu 2 O based photocathodes. Here, femtosecond time-resolved two-photon photoemission spectroscopy has been used to probe the electronic structure and dynamics of photoexcited charge carriers at the Cu 2 O surface as well as the interface between Cu 2 O and a platinum (Pt) adlayer. By referencing ultrafast energy-resolved surface sensitive spectroscopy to bulk data we identify the full bulk to surface transport dynamics for excited electrons rapidly localized within an intrinsic deep continuous defect band ranging from the whole crystal volume to the surface. No evidence of bulk electrons reaching the surface at the conduction band level is found resulting into a substantial loss of their energy through ultrafast trapping. Our results uncover main factors limiting the energy conversion processes in Cu 2 O and provide guidance for future material development.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); German Research Foundation (DFG)
- OSTI Identifier:
- 1619475
- Alternate Identifier(s):
- OSTI ID: 1559216
- Grant/Contract Number:
- AC02-05CH11231; SC0004993
- Resource Type:
- Published Article
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Name: Nature Communications Journal Volume: 10 Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Borgwardt, Mario, Omelchenko, Stefan T., Favaro, Marco, Plate, Paul, Höhn, Christian, Abou-Ras, Daniel, Schwarzburg, Klaus, van de Krol, Roel, Atwater, Harry A., Lewis, Nathan S., Eichberger, Rainer, and Friedrich, Dennis. Femtosecond time-resolved two-photon photoemission studies of ultrafast carrier relaxation in Cu2O photoelectrodes. United Kingdom: N. p., 2019.
Web. doi:10.1038/s41467-019-10143-x.
Borgwardt, Mario, Omelchenko, Stefan T., Favaro, Marco, Plate, Paul, Höhn, Christian, Abou-Ras, Daniel, Schwarzburg, Klaus, van de Krol, Roel, Atwater, Harry A., Lewis, Nathan S., Eichberger, Rainer, & Friedrich, Dennis. Femtosecond time-resolved two-photon photoemission studies of ultrafast carrier relaxation in Cu2O photoelectrodes. United Kingdom. https://doi.org/10.1038/s41467-019-10143-x
Borgwardt, Mario, Omelchenko, Stefan T., Favaro, Marco, Plate, Paul, Höhn, Christian, Abou-Ras, Daniel, Schwarzburg, Klaus, van de Krol, Roel, Atwater, Harry A., Lewis, Nathan S., Eichberger, Rainer, and Friedrich, Dennis. Wed .
"Femtosecond time-resolved two-photon photoemission studies of ultrafast carrier relaxation in Cu2O photoelectrodes". United Kingdom. https://doi.org/10.1038/s41467-019-10143-x.
@article{osti_1619475,
title = {Femtosecond time-resolved two-photon photoemission studies of ultrafast carrier relaxation in Cu2O photoelectrodes},
author = {Borgwardt, Mario and Omelchenko, Stefan T. and Favaro, Marco and Plate, Paul and Höhn, Christian and Abou-Ras, Daniel and Schwarzburg, Klaus and van de Krol, Roel and Atwater, Harry A. and Lewis, Nathan S. and Eichberger, Rainer and Friedrich, Dennis},
abstractNote = {Abstract Cuprous oxide (Cu 2 O) is a promising material for solar-driven water splitting to produce hydrogen. However, the relatively small accessible photovoltage limits the development of efficient Cu 2 O based photocathodes. Here, femtosecond time-resolved two-photon photoemission spectroscopy has been used to probe the electronic structure and dynamics of photoexcited charge carriers at the Cu 2 O surface as well as the interface between Cu 2 O and a platinum (Pt) adlayer. By referencing ultrafast energy-resolved surface sensitive spectroscopy to bulk data we identify the full bulk to surface transport dynamics for excited electrons rapidly localized within an intrinsic deep continuous defect band ranging from the whole crystal volume to the surface. No evidence of bulk electrons reaching the surface at the conduction band level is found resulting into a substantial loss of their energy through ultrafast trapping. Our results uncover main factors limiting the energy conversion processes in Cu 2 O and provide guidance for future material development.},
doi = {10.1038/s41467-019-10143-x},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United Kingdom},
year = {Wed May 08 00:00:00 EDT 2019},
month = {Wed May 08 00:00:00 EDT 2019}
}
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https://doi.org/10.1038/s41467-019-10143-x
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