Zhang, Xingfan;
Liu, Taifeng;
Zhu, Lei;
Guan, Jingcheng;
Lu, You;
Keal, Thomas W;
Buckeridge, John;
... Sokol, Alexey A; + view all
(2023)
Bulk and Surface Contributions to Ionisation Potentials of Metal Oxides.
Angewandte Chemie International Edition
, Article e202308411. 10.1002/anie.202308411.
(In press).
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Abstract
Determining the absolute band edge positions in solid materials is crucial for optimising their performance in wide-ranging applications including photocatalysis and electronic devices. However, obtaining absolute energies is challenging, as seen in CeO2, where experimental measurements show substantial discrepancies in the ionisation potential (IP). Here, we have combined several theoretical approaches, from classical electrostatics to quantum mechanics, to elucidate the bulk and surface contributions to the IP of metal oxides. We have determined a theoretical bulk contribution to the IP of stoichiometric CeO2 of only 5.38 eV, while surface orientation results in intrinsic IP variations from 4.2 eV to 8.2 eV. Highly tuneable IPs were also found in TiO2, ZrO2, and HfO2, in which surface polarisation plays a pivotal role in long-range energy level shifting. Our analysis, in addition to rationalising the observed range of experimental results, provides a firm basis for future interpretations of experimental and computational studies of oxide band structures.
| Type: | Article |
|---|---|
| Title: | Bulk and Surface Contributions to Ionisation Potentials of Metal Oxides |
| Location: | Germany |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/anie.202308411 |
| Publisher version: | https://doi.org/10.1002/anie.202308411 |
| Language: | English |
| Additional information: | © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/). |
| Keywords: | metal oxides, ionization potential, ceria, surface chemistry, QM/MM |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10175964 |
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