Morita, Kazuki;
Golomb, Matthias J;
Rivera, Miguel;
Walsh, Aron;
(2023)
Models of Polaron Transport in Inorganic and Hybrid Organic-Inorganic Titanium Oxides.
Chemistry of Materials
, 35
(9)
pp. 3652-3659.
10.1021/acs.chemmater.3c00322.
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Abstract
Polarons are a type of localized excess charge in materials and often form in transition metal oxides. The large effective mass and confined nature of polarons make them of fundamental interest for photochemical and electrochemical reactions. The most studied polaronic system is rutile TiO2 where electron addition results in small polaron formation through the reduction of Ti(IV) d0 to Ti(III) d1 centers. Using this model system, we perform a systematic analysis of the potential energy surface based on semiclassical Marcus theory parametrized from the first-principles potential energy landscape. We show that F-doped TiO2 only binds polaron weakly with effective dielectric screening after the second nearest neighbor. To tailor the polaron transport, we compare TiO2 to two metal-organic frameworks (MOFs): MIL-125 and ACM-1. The choice of MOF ligands and connectivity of the TiO6 octahedra largely vary the shape of the diabatic potential energy surface and the polaron mobility. Our models are applicable to other polaronic materials.
| Type: | Article |
|---|---|
| Title: | Models of Polaron Transport in Inorganic and Hybrid Organic-Inorganic Titanium Oxides |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acs.chemmater.3c00322 |
| Publisher version: | https://doi.org/10.1021/acs.chemmater.3c00322 |
| Language: | English |
| Additional information: | This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third-party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
| Keywords: | Science & Technology, Physical Sciences, Technology, Chemistry, Physical, Materials Science, Multidisciplinary, Chemistry, Materials Science, TOTAL-ENERGY CALCULATIONS, EXCESS ELECTRONS, RUTILE, ANATASE, TIO2, PHOTOCATALYSIS, CRYSTALLINE, FUNCTIONALS, EFFICIENCY, FRAMEWORKS |
| 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.ucl.ac.uk/id/eprint/10169773 |
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