Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors

Xia, Chelsea Q.; Peng, Jiali; Poncé, Samuel; Patel, Jay B.; Wright, Adam D.; Crothers, Timothy W.; Uller Rothmann, Mathias; Borchert, Juliane; Milot, Rebecca L.; Kraus, Hans; Lin, Qianqian; Giustino, Feliciano; Herz, Laura M.; Johnston, Michael B.

doi:10.1021/acs.jpclett.1c00619

Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors

Journal Article · Tue Apr 06 00:00:00 EDT 2021 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.1c00619· OSTI ID:1816735

Xia, Chelsea Q. ^[1]; Peng, Jiali ^[2]; ^[3]; ^[4]; ^[4]; Crothers, Timothy W. ^[4]; Uller Rothmann, Mathias ^[4]; ^[4]; ^[5]; Kraus, Hans ^[6]; ^[2]; ^[7]; ^[4]; ^[4]

Univ. of Oxford (United Kingdom). Clarendon Lab. Dept. of Physics; OSTI
Wuhan Univ. (China). School of Physics and Technology. Key Lab of Artificial Micro- and Nano-Structures of Ministry of Education of China
Univ. of Oxford (United Kingdom). Dept. of Materials; École Polytechnique Fédérale de Lausanne (Switzerland). Theory and Simulation of Materials (THEOS)
Univ. of Oxford (United Kingdom). Clarendon Lab. Dept. of Physics
Univ. of Warwick (United Kingdom). Dept. of Physics
Univ. of Oxford (United Kingdom). Dept. of Physics
Univ. of Oxford (United Kingdom). Dept. of Materials; Univ. of Texas, Austin, TX (United States). Oden Inst. for Computational Engineering and Sciences; Univ. of Texas, Austin, TX (United States). Dept. of Physics

Semiconducting polycrystalline thin films are cheap to produce and can be deposited on flexible substrates, yet high-performance electronic devices usually utilize single crystal 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.

View Accepted Manuscript (DOE)

Sponsoring Organization:: Marie Sklodowska-Curie Grant; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0020129

OSTI ID:: 1816735

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 14 Vol. 12; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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