Low-frequency optical phonon modes and carrier mobility in the halide perovskite CH3NH3PbBr3 using terahertz time-domain spectroscopy

Daming Zhao; Jonathan M. Skelton; Hongwei Hu; Chan La-O-Vorakiat; Jian Xin Zhu; Rudolph A. Marcus; Maria Elisabeth Michel-Beyerle; Yeng Ming Lam; Aron Walsh; Elbert E.M. Chia

doi:10.1063/1.4993524

Low-frequency optical phonon modes and carrier mobility in the halide perovskite CH₃NH₃PbBr₃ using terahertz time-domain spectroscopy

Daming Zhao, Jonathan M. Skelton, Hongwei Hu, Chan La-O-Vorakiat, Jian Xin Zhu, Rudolph A. Marcus, Maria Elisabeth Michel-Beyerle, Yeng Ming Lam, Aron Walsh, Elbert E.M. Chia

Department of Physics

Research output: Contribution to journal › Article › peer-review

56 Scopus citations

Abstract

As a light absorber in photovoltaic applications, hybrid organic-inorganic halide perovskites should have long and balanced diffusion lengths for both the separated electrons and holes before recombination, which necessitates high carrier mobility. In polar semiconductors, the roomerature carrier mobility is often limited by the scattering between carriers and the lowest-frequency optical phonon modes. Using terahertz time-domain spectroscopy, we examine the temperature evolution of these phonon modes in CH₃NH₃PbBr₃ and obtained high carrier mobility values using Feynman's polaron theory. This method allows us to estimate the upper limit of carrier mobilities without the need to create photogenerated free carriers, and can be applied to other heteropolar semiconductor systems with large polarons.

Original language	English
Article number	201903
Journal	Applied Physics Letters
Volume	111
Issue number	20
DOIs	https://doi.org/10.1063/1.4993524
State	Published - 13 Nov 2017

Bibliographical note

Funding Information:
D.M.Z. acknowledges support from TUM-CREATE. E.E.M.C. acknowledges support from the Singapore Ministry of Education AcRF Tier 1 (RG123/14) and Tier 2 (MOE2015-T2-2-065 and MOE2016-T2-1-054). C.L. acknowledges support from the Theoretical and Computational Science (TaCS) Center and Thailand Research Fund (MRG6080264). R.A.M. thanks the ONR and ARO for their support. M.-E.M.-B. is grateful to the Nanyang Technological University for supporting the Biophysics Center. The work was supported in part by the Center for Integrated Nanotechnologies, a U.S. DOE BES user facility. J.M.S. is grateful for support from the UK Engineering and Physical Sciences Research Council (EPSRC; Grant No. EP/P007821/1). Calculations were performed on the SiSu supercomputer at the IT Center for Science (CSC), Finland, via the Partnership for Advanced Computing in Europe (PRACE) Project No. 13DECI0317/ IsoSwitch.

Publisher Copyright:
© 2017 Author(s).

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Cite this

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title = "Low-frequency optical phonon modes and carrier mobility in the halide perovskite CH3NH3PbBr3 using terahertz time-domain spectroscopy",

abstract = "As a light absorber in photovoltaic applications, hybrid organic-inorganic halide perovskites should have long and balanced diffusion lengths for both the separated electrons and holes before recombination, which necessitates high carrier mobility. In polar semiconductors, the roomerature carrier mobility is often limited by the scattering between carriers and the lowest-frequency optical phonon modes. Using terahertz time-domain spectroscopy, we examine the temperature evolution of these phonon modes in CH3NH3PbBr3 and obtained high carrier mobility values using Feynman's polaron theory. This method allows us to estimate the upper limit of carrier mobilities without the need to create photogenerated free carriers, and can be applied to other heteropolar semiconductor systems with large polarons.",

author = "Daming Zhao and Skelton, {Jonathan M.} and Hongwei Hu and Chan La-O-Vorakiat and Zhu, {Jian Xin} and Marcus, {Rudolph A.} and Michel-Beyerle, {Maria Elisabeth} and Lam, {Yeng Ming} and Aron Walsh and Chia, {Elbert E.M.}",

note = "Funding Information: D.M.Z. acknowledges support from TUM-CREATE. E.E.M.C. acknowledges support from the Singapore Ministry of Education AcRF Tier 1 (RG123/14) and Tier 2 (MOE2015-T2-2-065 and MOE2016-T2-1-054). C.L. acknowledges support from the Theoretical and Computational Science (TaCS) Center and Thailand Research Fund (MRG6080264). R.A.M. thanks the ONR and ARO for their support. M.-E.M.-B. is grateful to the Nanyang Technological University for supporting the Biophysics Center. The work was supported in part by the Center for Integrated Nanotechnologies, a U.S. DOE BES user facility. J.M.S. is grateful for support from the UK Engineering and Physical Sciences Research Council (EPSRC; Grant No. EP/P007821/1). Calculations were performed on the SiSu supercomputer at the IT Center for Science (CSC), Finland, via the Partnership for Advanced Computing in Europe (PRACE) Project No. 13DECI0317/ IsoSwitch. Publisher Copyright: {\textcopyright} 2017 Author(s).",

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AU - Zhao, Daming

AU - Skelton, Jonathan M.

AU - Hu, Hongwei

AU - La-O-Vorakiat, Chan

AU - Zhu, Jian Xin

AU - Marcus, Rudolph A.

AU - Michel-Beyerle, Maria Elisabeth

AU - Lam, Yeng Ming

AU - Walsh, Aron

AU - Chia, Elbert E.M.

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PY - 2017/11/13

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N2 - As a light absorber in photovoltaic applications, hybrid organic-inorganic halide perovskites should have long and balanced diffusion lengths for both the separated electrons and holes before recombination, which necessitates high carrier mobility. In polar semiconductors, the roomerature carrier mobility is often limited by the scattering between carriers and the lowest-frequency optical phonon modes. Using terahertz time-domain spectroscopy, we examine the temperature evolution of these phonon modes in CH3NH3PbBr3 and obtained high carrier mobility values using Feynman's polaron theory. This method allows us to estimate the upper limit of carrier mobilities without the need to create photogenerated free carriers, and can be applied to other heteropolar semiconductor systems with large polarons.

AB - As a light absorber in photovoltaic applications, hybrid organic-inorganic halide perovskites should have long and balanced diffusion lengths for both the separated electrons and holes before recombination, which necessitates high carrier mobility. In polar semiconductors, the roomerature carrier mobility is often limited by the scattering between carriers and the lowest-frequency optical phonon modes. Using terahertz time-domain spectroscopy, we examine the temperature evolution of these phonon modes in CH3NH3PbBr3 and obtained high carrier mobility values using Feynman's polaron theory. This method allows us to estimate the upper limit of carrier mobilities without the need to create photogenerated free carriers, and can be applied to other heteropolar semiconductor systems with large polarons.

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