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Electron Localization in Defective Ceria Films: A Study with Scanning-Tunneling Microscopy and Density-Functional Theory

Jan-Frederik Jerratsch, Xiang Shao, Niklas Nilius, Hans-Joachim Freund, Cristina Popa, M. Veronica Ganduglia-Pirovano, Asbjörn M. Burow, and Joachim Sauer
Phys. Rev. Lett. 106, 246801 – Published 14 June 2011

Abstract

Scanning-tunneling microscopy and density-functional theory have been employed to identify the spatial correlation between an oxygen vacancy and the associated Ce3+ ion pair in a defective CeO2(111) film. The two Ce3+ ions can occupy different cationic shells around the vacancy. The resulting variation in the chemical environment leads to a splitting of the filled Ce3+ f levels, which is detected with STM spectroscopy. The position of the Ce3+ ion pair is reflected in characteristic defect patterns observed in empty-state STM images, which arise from the bright appearance of Ce4+ ions next to the defect while the Ce3+ remain dark. Both findings demonstrate that at least one excess electron localizes in a Ce ion that is not adjacent to the O vacancy.

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  • Received 5 January 2011

DOI:https://doi.org/10.1103/PhysRevLett.106.246801

© 2011 American Physical Society

Authors & Affiliations

Jan-Frederik Jerratsch1, Xiang Shao1, Niklas Nilius1,*, Hans-Joachim Freund1, Cristina Popa2, M. Veronica Ganduglia-Pirovano2,†, Asbjörn M. Burow2, and Joachim Sauer2,‡

  • 1Fritz-Haber-Institut der MPG, Faradayweg 4-6, 14195 Berlin, Germany
  • 2Humboldt-Universität zu Berlin, Unter den Linden 6, 10099 Berlin, Germany

  • *Corresponding author. nilius@fhi-berlin.mpg.de
  • Present address: Institute of Catalysis and Petrochemistry-CSIC, Marie Curie 2, 28049 Madrid, Spain.
  • Corresponding author. js@chemie.hu-berlin.de

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Issue

Vol. 106, Iss. 24 — 17 June 2011

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