In situ observation of picosecond polaron self-localisation in α-Fe2O3 photoelectrochemical cells

Ernest Pastor (), Ji-Sang Park, Ludmilla Steier, Sunghyun Kim, Michael Grätzel, James R. Durrant, Aron Walsh and Artem A. Bakulin
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Ernest Pastor: Imperial College London
Ji-Sang Park: Imperial College London
Ludmilla Steier: Imperial College London
Sunghyun Kim: Imperial College London
Michael Grätzel: Ecole Polytechnique Fédérale de Lausanne, Institut des Sciences et Ingénierie Chimiques
James R. Durrant: Imperial College London
Aron Walsh: Imperial College London
Artem A. Bakulin: Imperial College London

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract Hematite (α-Fe2O3) is the most studied artificial oxygen-evolving photo-anode and yet its efficiency limitations and their origin remain unknown. A sub-picosecond reorganisation of the hematite structure has been proposed as the mechanism which dictates carrier lifetimes, energetics and the ultimate conversion yields. However, the importance of this reorganisation for actual device performance is unclear. Here we report an in situ observation of charge carrier self-localisation in a hematite device, and demonstrate that this process affects recombination losses in photoelectrochemical cells. We apply an ultrafast, device-based optical-control method to resolve the subpicosecond formation of small polarons and estimate their reorganisation energy to be ~0.5 eV. Coherent oscillations in the photocurrent signals indicate that polaron formation may be coupled to specific phonon modes (

Date: 2019
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DOI: 10.1038/s41467-019-11767-9

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