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Issue 7, 2019
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Charge carrier dynamics in tantalum oxide overlayered and tantalum doped hematite photoanodes

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Abstract

We employ atomic layer deposition to prepare 50 nm thick hematite photoanodes followed by passivating them with a 0.5 nm thick Ta2O5-overlayer and compare them with samples uniformly doped with the same amount of tantalum. We observe a three-fold improvement in photocurrent with the same onset voltage using Ta-overlayer hematite photoanodes, while electrochemical impedance spectroscopy under visible light irradiation shows a decreased amount of surface states under water splitting conditions. The Ta-doped samples have an even higher increase in photocurrent along with a 0.15 V cathodic shift in the onset voltage and decreased resistivity. However, the surface state capacitance for the Ta-doped sample is twice that of the reference photoanode, which implies a larger amount of surface hole accumulation. We further utilize transient absorption spectroscopy in the sub-millisecond to second timescale under operating conditions to show that electron trapping in both Ta2O5-passivated and Ta-doped samples is markedly reduced. Ultrafast transient absorption spectroscopy in the sub-picosecond to nanosecond timescale shows faster charge carrier dynamics and reduced recombination in the Ta-doped hematite photoanode resulting in the increased photoelectrochemical performance when compared with the Ta2O5-overlayer sample. Our results show that passivation does not affect the poor charge carrier dynamics intrinsic to hematite based photoanodes. The Ta-doping strategy results in more efficient electron extraction, solving the electron trapping issue and leading to increased performance over the surface passivation strategy.

Graphical abstract: Charge carrier dynamics in tantalum oxide overlayered and tantalum doped hematite photoanodes

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Supplementary files

Article information


Submitted
01 Oct 2018
Accepted
14 Jan 2019
First published
14 Jan 2019

This article is Open Access

J. Mater. Chem. A, 2019,7, 3206-3215
Article type
Paper

Charge carrier dynamics in tantalum oxide overlayered and tantalum doped hematite photoanodes

T. Ruoko, A. Hiltunen, T. Iivonen, R. Ulkuniemi, K. Lahtonen, H. Ali-Löytty, K. Mizohata, M. Valden, M. Leskelä and N. V. Tkachenko, J. Mater. Chem. A, 2019, 7, 3206
DOI: 10.1039/C8TA09501A

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