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Direct observation of the energetics at a semiconductor/liquid junction by operando X-ray photoelectron spectroscopy

Lichterman, Michael F. and Hu, Shu and Richter, Matthias H. and Crumlin, Ethan J. and Axnanda, Stephanus and Favaro, Marco and Drisdell, Walter and Hussain, Zahid and Mayer, Thomas and Brunschwig, Bruce S. and Lewis, Nathan S. and Liu, Zhi and Lewerenz, Hans-Joachim (2015) Direct observation of the energetics at a semiconductor/liquid junction by operando X-ray photoelectron spectroscopy. Energy and Environmental Science, 8 (8). pp. 2409-2416. ISSN 1754-5692. doi:10.1039/C5EE01014D.

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Photoelectrochemical (PEC) cells based on semiconductor/liquid interfaces provide a method of converting solar energy to electricity or fuels. Currently, the understanding of semiconductor/liquid interfaces is inferred from experiments and models. Operando ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) has been used herein to directly characterize the semiconductor/liquid junction at room temperature under real-time electrochemical control. X-ray synchrotron radiation in conjunction with AP-XPS has enabled simultaneous monitoring of the solid surface, the solid/electrolyte interface, and the bulk electrolyte of a PEC cell as a function of the applied potential, U. The observed shifts in binding energy with respect to the applied potential have directly revealed ohmic and rectifying junction behavior on metallized and semiconducting samples, respectively. Additionally, the non-linear response of the core level binding energies to changes in the applied electrode potential has revealed the influence of defect-derived electronic states on the Galvani potential across the complete cell.

Item Type:Article
Related URLs:
URLURL TypeDescription DOIArticle
Lichterman, Michael F.0000-0002-0710-7068
Hu, Shu0000-0002-5041-0169
Richter, Matthias H.0000-0003-0091-2045
Crumlin, Ethan J.0000-0003-3132-190X
Drisdell, Walter0000-0002-8693-4562
Brunschwig, Bruce S.0000-0002-6135-6727
Lewis, Nathan S.0000-0001-5245-0538
Lewerenz, Hans-Joachim0000-0001-8433-9471
Additional Information:© 2015 Royal Society of Chemistry. Received 30th March 2015; accepted 29th May 2015. First published online 29 May 2015. This work was supported through the Office of Science of the U.S. Department of Energy (DOE) under award no. DE-SC0004993 to the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. We acknowledge Dr. Philip Ross for his contributions to the conceptual development of the AP-XPS endstation and experimental design, and Junko Yano for fruitful discussions. We acknowledge Fadl Saadi, Beomgyun Jeong, and Sana Rani for assistance during data collection at the beamline.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
Issue or Number:8
Record Number:CaltechAUTHORS:20150706-104957791
Persistent URL:
Official Citation:Lichterman, M. F., Hu, S., Richter, M. H., Crumlin, E. J., Axnanda, S., Favaro, M., . . . Lewerenz, H.-J. (2015). Direct observation of the energetics at a semiconductor/liquid junction by operando X-ray photoelectron spectroscopy. [10.1039/C5EE01014D]. Energy & Environmental Science. doi: 10.1039/c5ee01014d
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:58774
Deposited On:06 Jul 2015 21:37
Last Modified:10 Nov 2021 22:10

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