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Correlated electron-nuclear dynamics of photoinduced water dissociation on rutile TiO 2 .
- Source :
-
Nature materials [Nat Mater] 2024 Aug; Vol. 23 (8), pp. 1100-1106. Date of Electronic Publication: 2024 May 22. - Publication Year :
- 2024
-
Abstract
- Elucidating the mechanism of photoinduced water splitting on TiO <subscript>2</subscript> is important for advancing the understanding of photocatalysis and the ability to control photocatalytic surface reactions. However, incomplete experimental information and complex coupled electron-nuclear motion make the microscopic understanding challenging. Here we analyse the atomic-scale pathways of photogenerated charge carrier transport and photoinduced water dissociation at the prototypical water-rutile TiO <subscript>2</subscript> (110) interface using first-principles dynamics simulations. Two distinct mechanisms are observed. Field-initiated electron migration leads to adsorbed water dissociation via proton transfer to a surface bridging oxygen. In the other pathway, adsorbed water dissociation occurs via proton donation to a second-layer water molecule coupled to photoexcited-hole transfer promoted by in-plane surface lattice distortions. Two stages of non-adiabatic in-plane lattice motion-expansion and recovery-are observed, which are closely associated with population changes in Ti3d orbitals. Controlling such highly correlated electron-nuclear dynamics may provide opportunities for boosting the performance of photocatalytic materials.<br /> (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)
Details
- Language :
- English
- ISSN :
- 1476-4660
- Volume :
- 23
- Issue :
- 8
- Database :
- MEDLINE
- Journal :
- Nature materials
- Publication Type :
- Academic Journal
- Accession number :
- 38777872
- Full Text :
- https://doi.org/10.1038/s41563-024-01900-5