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Evolution of the electronic structure of CaO thin films following Mo interdiffusion at high temperature

MPS-Authors
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Cui,  Yi
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Pan,  Yi
Chemical Physics, Fritz Haber Institute, Max Planck Society;
Paul-Drude-Institut für Festkörperelektronik;

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Pascua,  Leandro
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Qiu,  Hengshan
Chemical Physics, Fritz Haber Institute, Max Planck Society;
Xinjiang Technical Institute of Physics and Chemistry of CAS;

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Stiehler,  Christian
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Kuhlenbeck,  Helmut
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Freund,  Hans-Joachim
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Fulltext (public)

PhysRevB.91.035418.pdf
(Publisher version), 2MB

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Citation

Cui, Y., Pan, Y., Pascua, L., Qiu, H., Stiehler, C., Kuhlenbeck, H., et al. (2015). Evolution of the electronic structure of CaO thin films following Mo interdiffusion at high temperature. Physical Review B, 91(3): 035418. doi:10.1103/PhysRevB.91.035418.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0024-AD38-B
Abstract
The electronic structure of CaO films of 10–60 monolayer thickness grown on Mo(001) has been investigated with synchrotron-mediated x-ray photoelectron spectroscopy (XPS) and scanning tunneling microscopy (STM). Upon annealing or reducing the thickness of the film, a rigid shift of the CaO bands to lower energy is revealed. This evolution is explained with a temperature-induced diffusion of Mo ions from the metal substrate to the oxide and their accumulation in the interface region of the film. The Mo substitutes divalent Ca species in the rocksalt lattice and is able to release electrons to the system. The subsequent changes in the Mo oxidation state have been followed with high-resolution XPS measurements. While near-interface Mo transfers extra electrons back to the substrate, generating an interface dipole that gives rise to the observed band shift, near-surface species are able to exchange electrons with adsorbates bound to the oxide surface. For example, exposure of O2 results in the formation of superoxo species on the oxide surface, as revealed from STM measurements. Mo interdiffusion is therefore responsible for the pronounced donor character of the initially inert oxide, and largely modifies its adsorption and reactivity behavior.