Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy

Thomas J. Penfold, Jakub Szlachetko, Fabio G. Santomauro, Alexander Britz, Wojciech Gawelda, Gilles Doumy, Anne Marie March, Stephen H. Southworth, Jochen Rittmann, Rafael Abela, Majed Chergui and Christopher J. Milne ()
Additional contact information
Thomas J. Penfold: Newcastle University
Jakub Szlachetko: Paul Scherrer Institut
Fabio G. Santomauro: FSB and Lausanne Centre for Ultrafast Science (LACUS)
Alexander Britz: European XFEL
Wojciech Gawelda: European XFEL
Gilles Doumy: Argonne National Laboratory
Anne Marie March: Argonne National Laboratory
Stephen H. Southworth: Argonne National Laboratory
Jochen Rittmann: FSB and Lausanne Centre for Ultrafast Science (LACUS)
Rafael Abela: Paul Scherrer Institut
Majed Chergui: FSB and Lausanne Centre for Ultrafast Science (LACUS)
Christopher J. Milne: Paul Scherrer Institut

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract Nanostructures of transition metal oxides, such as zinc oxide, have attracted considerable interest for solar-energy conversion and photocatalysis. Both applications are sensitive to the transport and trapping of photoexcited charge carriers. The probing of electron trapping has recently become possible using time-resolved element-sensitive methods, such as X-ray spectroscopy. However, valence-band-trapped holes have so far escaped observation. Herein we use X-ray absorption spectroscopy combined with a dispersive X-ray emission spectrometer to probe the charge carrier relaxation and trapping processes in zinc oxide nanoparticles after above band-gap photoexcitation. Our results, supported by simulations, demonstrate that within 80 ps, photoexcited holes are trapped at singly charged oxygen vacancies, which causes an outward displacement by ~15% of the four surrounding zinc atoms away from the doubly charged vacancy. This identification of the hole traps provides insight for future developments of transition metal oxide-based nanodevices.

Date: 2018
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DOI: 10.1038/s41467-018-02870-4

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