Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors

Xia, Chelsea Q.;Peng, Jiali;Poncé, Samuel;Patel, Jay B.;Johnston, Michael B.;et.al.
(2021) Journal of Physical Chemistry Letters — Vol. 12, n° 14, p. 3607-3617 (2021)

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Authors
  • Xia, Chelsea Q.Department of Physics, University of Oxford, Clarendon Laboratory, Oxford OX1 3PU, U.K.
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  • Peng, JialiKey Lab of Artificial Micro- and Nano-Structures of Ministry of Education of China, School of Physics and Technology, Wuhan University, Wuhan 430072, P.R. China
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  • Poncé, Samuelorcid-logoUCLouvain
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  • Patel, Jay B.orcid-logoDepartment of Physics, University of Oxford, Clarendon Laboratory, Oxford OX1 3PU, U.K.
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  • Johnston, Michael B.orcid-logoDepartment of Physics, University of Oxford, Clarendon Laboratory, Oxford OX1 3PU, U.K.;
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Abstract
Semiconducting polycrystalline thin films are cheap to produce and can be deposited on flexible substrates, yet high-performance electronic devices usually utilize singlecrystal semiconductors, owing to their superior charge-carrier mobilities and longer diffusion lengths. Here we show that the electrical performance of polycrystalline films of metal-halide perovskites (MHPs) approaches that of single crystals at room temperature. Combining temperature-dependent terahertz conductivity measurements and ab initio calculations we uncover a complete picture of the origins of charge-carrier scattering in single crystals and polycrystalline films of CH3NH3PbI3. We show that Fröhlich scattering of charge carriers with multiple phonon modes is the dominant mechanism limiting mobility, with grain-boundary scattering further reducing mobility in polycrystalline films. We reconcile the large discrepancy in charge-carrier diffusion lengths between single crystals and films by considering photon reabsorption. Thus, polycrystalline films of MHPs offer great promise for devices beyond solar cells, including light-emitting diodes and modulators.
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Xia, C. Q., Peng, J., Poncé, S., Patel, J. B., Wright, A. D., Crothers, T. W., Uller Rothmann, M., Borchert, J., Milot, R. L., Kraus, H., Lin, Q., Giustino, F., Herz, L. M., & Johnston, M. B. (2021). Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors. Journal of Physical Chemistry Letters, 12(14), 3607-3617. https://doi.org/10.1021/acs.jpclett.1c00619 (Original work published 2021)