High carrier mobility along the [111] orientation in Cu2O photoelectrodes

Linfeng Pan, Linjie Dai, Oliver J. Burton, Lu Chen, Virgil Andrei, Youcheng Zhang, Dan Ren, Jinshui Cheng, Linxiao Wu, Kyle Frohna, Anna Abfalterer, Terry Chien-Jen Yang, Wenzhe Niu, Meng Xia, Stephan Hofmann, Paul J. Dyson, Erwin Reisner, Henning Sirringhaus, Jingshan Luo (), Anders Hagfeldt (), Michael Grätzel () and Samuel D. Stranks ()
Additional contact information
Linfeng Pan: University of Cambridge
Linjie Dai: University of Cambridge
Oliver J. Burton: University of Cambridge
Lu Chen: École Polytechnique Fédérale de Lausanne
Virgil Andrei: University of Cambridge
Youcheng Zhang: University of Cambridge
Dan Ren: École Polytechnique Fédérale de Lausanne
Jinshui Cheng: Nankai University
Linxiao Wu: Nankai University
Kyle Frohna: University of Cambridge
Anna Abfalterer: University of Cambridge
Terry Chien-Jen Yang: University of Cambridge
Wenzhe Niu: École Polytechnique Fédérale de Lausanne
Meng Xia: École Polytechnique Fédérale de Lausanne
Stephan Hofmann: University of Cambridge
Paul J. Dyson: École Polytechnique Fédérale de Lausanne
Erwin Reisner: University of Cambridge
Henning Sirringhaus: University of Cambridge
Jingshan Luo: Nankai University
Anders Hagfeldt: École Polytechnique Fédérale de Lausanne
Michael Grätzel: École Polytechnique Fédérale de Lausanne
Samuel D. Stranks: University of Cambridge

Nature, 2024, vol. 628, issue 8009, 765-770

Abstract: Abstract Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight1,2. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials3–5. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance6. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111] direction was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm−2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h.

Date: 2024
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DOI: 10.1038/s41586-024-07273-8

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