Milot, Rebecca L., Eperon, Giles E., Snaith, Henry J., Johnston, Michael B. and Herz, Laura M. (2015) Temperature-dependent charge-carrier dynamics in CH3NH3PbI3 perovskite thin films. Advanced Functional Materials, 25 (39). pp. 6218-6227. doi:10.1002/adfm.201502340 ISSN 1616-301X.

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Abstract

The photoluminescence, transmittance, charge‐carrier recombination dynamics, mobility, and diffusion length of CH3NH3PbI3 are investigated in the temperature range from 8 to 370 K. Profound changes in the optoelectronic properties of this prototypical photovoltaic material are observed across the two structural phase transitions occurring at 160 and 310 K. Drude‐like terahertz photoconductivity spectra at all temperatures above 80 K suggest that charge localization effects are absent in this range. The monomolecular charge‐carrier recombination rate generally increases with rising temperature, indicating a mechanism dominated by ionized impurity mediated recombination. Deduced activation energies Ea associated with ionization are found to increase markedly from the room‐temperature tetragonal (Ea ≈ 20 meV) to the higher‐temperature cubic (Ea ≈ 200 meV) phase adopted above 310 K. Conversely, the bimolecular rate constant decreases with rising temperature as charge‐carrier mobility declines, while the Auger rate constant is highly phase specific, suggesting a strong dependence on electronic band structure. The charge‐carrier diffusion length gradually decreases with rising temperature from about 3 μm at −93 °C to 1.2 μm at 67 °C but remains well above the optical absorption depth in the visible spectrum. These results demonstrate that there are no fundamental obstacles to the operation of cells based on CH3NH3PbI3 under typical field conditions.

Item Type:	Journal Article
Subjects:	Q Science > QC Physics
Divisions:	Faculty of Science, Engineering and Medicine > Science > Physics
Journal or Publication Title:	Advanced Functional Materials
Publisher:	Wiley - V C H Verlag GmbH & Co. KGaA
ISSN:	1616-301X
Official Date:	15 October 2015
Dates:	Date Event 15 October 2015 Published 15 September 2015 Available 24 July 2015 Accepted 9 June 2015 Submitted
Volume:	25
Number:	39
Page Range:	pp. 6218-6227
DOI:	10.1002/adfm.201502340
Status:	Peer Reviewed
Publication Status:	Published
Access rights to Published version:	Open Access (Creative Commons)
Date of first compliant deposit:	30 July 2019
Date of first compliant Open Access:	30 July 2019
RIOXX Funder/Project Grant:	Project/Grant ID RIOXX Funder Name Funder ID UNSPECIFIED [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266

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