Imperial College London

Professor James Durrant, CBE, FRS

Faculty of Natural SciencesDepartment of Chemistry

Professor of Photochemistry
 
 
 
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Contact

 

+44 (0)20 7594 5321j.durrant Website

 
 
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Assistant

 

Miss Lisa Benbow +44 (0)20 7594 5883

 
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Location

 

G22CMolecular Sciences Research HubWhite City Campus

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Summary

 

Publications

Citation

BibTex format

@article{Bakulin:2019:10.1038/s41467-019-11767-9,
author = {Bakulin, A and Pastor, E and Park, J-S and Steier, L and Kim, S and Grätzel, M and Durrant, J and Walsh, A},
doi = {10.1038/s41467-019-11767-9},
journal = {Nature Communications},
title = {In situ observation of picosecond polaron self-localisation in α-Fe2O3 photoelectrochemical cells},
url = {http://dx.doi.org/10.1038/s41467-019-11767-9},
volume = {10},
year = {2019}
}

RIS format (EndNote, RefMan)

TY  - JOUR
AB - 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 (<100 cm-1). Our results bring together spectroscopic and device characterisation approaches to reveal new photophysics of broadly-studied hematite devices.
AU - Bakulin,A
AU - Pastor,E
AU - Park,J-S
AU - Steier,L
AU - Kim,S
AU - Grätzel,M
AU - Durrant,J
AU - Walsh,A
DO - 10.1038/s41467-019-11767-9
PY - 2019///
SN - 2041-1723
TI - In situ observation of picosecond polaron self-localisation in α-Fe2O3 photoelectrochemical cells
T2 - Nature Communications
UR - http://dx.doi.org/10.1038/s41467-019-11767-9
UR - http://hdl.handle.net/10044/1/72569
VL - 10
ER -