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We report the experimental observation and theoretical explanation of an unconventional interplay between divalent Co and trivalent Y dopants, both of which incur oxygen vacancies in the CeO 2  host that has predominantly tetravalent Ce cations. The Co dopant atoms were experimentally found to act as a switch that turns on the dormant effect of Y-modulated band-gap reduction. As revealed by density functional theory (DFT) calculations with structures verified by synchrotron-radiation x-ray measurements, a Co 3d band that hybridizes with Ce 4f band was lowered due to reduced O 2p repulsion arising from oxygen vacancies incurred by Y doping and therefore gave rise to the observed band-gap narrowing effect. Such switch-and-modulator scheme for band-gap engineering in nanocrystal materials can lead to important applications in environmental protection and solar energy harvesting technologies.

Unconventional interplay between heterovalent dopant elements: Switch-and-modulator band-gap engineering in (Y, Co)-Codoped CeO2 nanocrystals