Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy
Abstract
Nanostructures of transition metal oxides (TMO), such as ZnO, have attracted considerable interest for solar-energy conversion and photocatalysis. For the latter, trapping of charge carriers has an essential role. The probing of electron trapping in the conduction band of room temperature photoexcited TMOs has recently become possible owing to the emergence of time-resolved element-sensitive methods, such as X-ray spectroscopy. However, because the valence band of TMOs is dominated by the oxygen 2p orbitals,holes have so far escaped observation. Herein we use a novel dispersive X-ray emission spectrometer combined with X-ray absorption spectroscopy to directly probe the charge carrier relaxation and trapping pro-cesses in ZnO nanoparticles after above band-gap photoexcitation. Here, our results, supported by simulations, demonstrate that within our temporal resolution of 80 ps, photo-excited holes are trapped at singly charged oxygen vacancies, turning them into doubly charged vacancies, which causes an outward displacement by approximately 15% of the four surrounding Zn atoms away from the central vacancy. These traps recombine radiatively with the delocalised electrons of the conduction band yielding the commonly observed green luminescence. This identification of the hole traps and their evolution provides new insight for future developments of TMO-based nanodevices.
- Authors:
-
- Newcastle Univ., Newcastle upon Tyne (United Kingdom). Chemistry-School of Natural and Environmental Sciences
- Paul Scherrer Inst. (PSI), Villigen (Switzerland). SwissFEL; Polish Academy of Sciences (PAS), Krakow (Poland). Inst. of Nuclear Physics
- Ecole Polytechnique Federale Lausanne (Switzlerland)
- European X-ray Free-Electron Laser (XFEL), Schenefeld (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
- European X-ray Free-Electron Laser (XFEL), Schenefeld (Germany); Adam Mickiewicz Univ., Poznan (Poland). Faculty of Physics
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Paul Scherrer Inst. (PSI), Villigen (Switzerland). SwissFEL
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Swiss National Science Foundation (SNSF); National Science Centre, Poland (NCN); German Research Foundation (DFG); European Research Council (ERC)
- OSTI Identifier:
- 1429363
- Grant/Contract Number:
- AC02-06CH11357; 2015/18/E/ST3/00444; 2016/ 22/E/ST4/00543
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; Nanoparticles; Optical materials; X-rays
Citation Formats
Penfold, Thomas J., Szlachetko, Jakub, Santomauro, Fabio G., Britz, Alexander, Gawelda, Wojciech, Doumy, Gilles, March, Anne Marie, Southworth, Stephen H., Rittmann, Jochen, Abela, Rafael, Chergui, Majed, and Milne, Christopher J. Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-02870-4.
Penfold, Thomas J., Szlachetko, Jakub, Santomauro, Fabio G., Britz, Alexander, Gawelda, Wojciech, Doumy, Gilles, March, Anne Marie, Southworth, Stephen H., Rittmann, Jochen, Abela, Rafael, Chergui, Majed, & Milne, Christopher J. Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy. United States. https://doi.org/10.1038/s41467-018-02870-4
Penfold, Thomas J., Szlachetko, Jakub, Santomauro, Fabio G., Britz, Alexander, Gawelda, Wojciech, Doumy, Gilles, March, Anne Marie, Southworth, Stephen H., Rittmann, Jochen, Abela, Rafael, Chergui, Majed, and Milne, Christopher J. Fri .
"Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy". United States. https://doi.org/10.1038/s41467-018-02870-4. https://www.osti.gov/servlets/purl/1429363.
@article{osti_1429363,
title = {Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy},
author = {Penfold, Thomas J. and Szlachetko, Jakub and Santomauro, Fabio G. and Britz, Alexander and Gawelda, Wojciech and Doumy, Gilles and March, Anne Marie and Southworth, Stephen H. and Rittmann, Jochen and Abela, Rafael and Chergui, Majed and Milne, Christopher J.},
abstractNote = {Nanostructures of transition metal oxides (TMO), such as ZnO, have attracted considerable interest for solar-energy conversion and photocatalysis. For the latter, trapping of charge carriers has an essential role. The probing of electron trapping in the conduction band of room temperature photoexcited TMOs has recently become possible owing to the emergence of time-resolved element-sensitive methods, such as X-ray spectroscopy. However, because the valence band of TMOs is dominated by the oxygen 2p orbitals,holes have so far escaped observation. Herein we use a novel dispersive X-ray emission spectrometer combined with X-ray absorption spectroscopy to directly probe the charge carrier relaxation and trapping pro-cesses in ZnO nanoparticles after above band-gap photoexcitation. Here, our results, supported by simulations, demonstrate that within our temporal resolution of 80 ps, photo-excited holes are trapped at singly charged oxygen vacancies, turning them into doubly charged vacancies, which causes an outward displacement by approximately 15% of the four surrounding Zn atoms away from the central vacancy. These traps recombine radiatively with the delocalised electrons of the conduction band yielding the commonly observed green luminescence. This identification of the hole traps and their evolution provides new insight for future developments of TMO-based nanodevices.},
doi = {10.1038/s41467-018-02870-4},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Fri Feb 02 00:00:00 EST 2018},
month = {Fri Feb 02 00:00:00 EST 2018}
}
Web of Science
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Origin of Visible Photoluminescence of ZnO Quantum Dots: Defect-Dependent and Size-Dependent
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Guest–Host Interactions Investigated by Time-Resolved X-ray Spectroscopies and Scattering at MHz Rates: Solvation Dynamics and Photoinduced Spin Transition in Aqueous Fe(bipy) 3 2+
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The Kinetics of the Radiative and Nonradiative Processes in Nanocrystalline ZnO Particles upon Photoexcitation
journal, March 2000
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Influence of Adsorbed Oxygen on the Emission Properties of Nanocrystalline ZnO Particles
journal, May 2000
- van Dijken, Addy; Meulenkamp, Eric A.; Vanmaekelbergh, Daniël
- The Journal of Physical Chemistry B, Vol. 104, Issue 18
Observation of Transient Iron(II) Formation in Dye-Sensitized Iron Oxide Nanoparticles by Time-Resolved X-ray Spectroscopy
journal, April 2010
- Katz, Jordan E.; Gilbert, Benjamin; Zhang, Xiaoyi
- The Journal of Physical Chemistry Letters, Vol. 1, Issue 9
Photoinduced Interfacial Electron Injection Dynamics in Dye-Sensitized Solar Cells under Photovoltaic Operating Conditions
journal, December 2012
- Teuscher, Joël; Décoppet, Jean-David; Punzi, Angela
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 24
Real Time Determination of the Electronic Structure of Unstable Reaction Intermediates during Au 2 O 3 Reduction
journal, December 2013
- Szlachetko, Jakub; Sá, Jacinto; Nachtegaal, Maarten
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 1
Ab Initio Thermodynamics of Oxygen Vacancies and Zinc Interstitials in ZnO
journal, November 2014
- Bjørheim, Tor S.; Kotomin, Eugene
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 24
Photocatalytic Degradation of Methyl Orange over Single Crystalline ZnO: Orientation Dependence of Photoactivity and Photostability of ZnO
journal, March 2009
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Femtosecond X-ray absorption study of electron localization in photoexcited anatase TiO2
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Oxygen vacancies in ZnO
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Modeling ZnO phases using a periodic approach: From bulk to surface and beyond
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Electron energy loss spectroscopy of ZnO nanocrystals with different oxygen vacancy concentrations
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Development of high-repetition-rate laser pump/x-ray probe methodologies for synchrotron facilities
journal, July 2011
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A von Hamos x-ray spectrometer based on a segmented-type diffraction crystal for single-shot x-ray emission spectroscopy and time-resolved resonant inelastic x-ray scattering studies
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journal, June 2017
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Femtosecond XANES Study of the Light-Induced Spin Crossover Dynamics in an Iron(II) Complex
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