Correlated electron-nuclear dynamics of photoinduced water dissociation on rutile TiO<sub>2</sub>.

You, Peiwei; Chen, Daqiang; Liu, Xinbao; Zhang, Cui; Selloni, Annabella; Meng, Sheng

Correlated electron-nuclear dynamics of photoinduced water dissociation on rutile TiO₂.

You, Peiwei; Chen, Daqiang; Liu, Xinbao; Zhang, Cui; Selloni, Annabella; Meng, Sheng.

Afiliación

You P; Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing, China.
Chen D; School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, China.
Liu X; Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing, China.
Zhang C; School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, China.
Selloni A; Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing, China.
Meng S; School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, China.

Nat Mater ; 23(8): 1100-1106, 2024 Aug.

Article en En | MEDLINE | ID: mdl-38777872

ABSTRACT

ABSTRACT

Elucidating the mechanism of photoinduced water splitting on TiO2 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 TiO2(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.

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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Mater Asunto de la revista: CIENCIA / QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Reino Unido

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