Femtosecond time-resolved two-photon photoemission studies of ultrafast carrier relaxation in Cu2O photoelectrodes

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

doi:10.1038/s41467-019-10143-x

Title: Femtosecond time-resolved two-photon photoemission studies of ultrafast carrier relaxation in Cu2O photoelectrodes

Journal Article · 08 May 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-10143-x · OSTI ID:1619475

; Omelchenko, Stefan T.; Favaro, Marco; Plate, Paul; Höhn, Christian; Abou-Ras, Daniel; Schwarzburg, Klaus;

;

; Eichberger, Rainer;

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.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0004993

OSTI ID:: 1619475

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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