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 room-temperature 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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13 November 2017
Research Article|
November 16 2017
Low-frequency optical phonon modes and carrier mobility in the halide perovskite CH3NH3PbBr3 using terahertz time-domain spectroscopy
Daming Zhao
;
Daming Zhao
1
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University
, Singapore
637371, Singapore
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Jonathan M. Skelton;
Jonathan M. Skelton
2
Department of Chemistry, University of Bath
, Claverton Down, Bath BA2 7AY, United Kingdom
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Hongwei Hu;
Hongwei Hu
3
School of Materials Science and Engineering, Nanyang Technological University
, Singapore
639798, Singapore
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Chan La-o-vorakiat;
Chan La-o-vorakiat
4
Nanoscience and Nanotechnology Graduate Program, King Mongkut's University of Technology Thonburi
, Bangkok 10140, Thailand
5
Theoretical and Computational Science Center (TaCS), Faculty of Science, King Mongkut's University of Technology Thonburi
, Bangkok 10140, Thailand
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Jian-Xin Zhu;
Jian-Xin Zhu
6
Theoretical Division, Los Alamos National Laboratory
, Los Alamos, New Mexico 87545, USA
7
Center for Integrated Nanotechnologies, Los Alamos National Laboratories
, Los Alamos, New Mexico 87545, USA
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Rudolph A. Marcus;
Rudolph A. Marcus
1
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University
, Singapore
637371, Singapore
8
Noyes Laboratory, California Institute of Technology
, Pasadena, California 91125, USA
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Maria-Elisabeth Michel-Beyerle;
Maria-Elisabeth Michel-Beyerle
1
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University
, Singapore
637371, Singapore
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Yeng Ming Lam;
Yeng Ming Lam
3
School of Materials Science and Engineering, Nanyang Technological University
, Singapore
639798, Singapore
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Aron Walsh
;
Aron Walsh
a)
2
Department of Chemistry, University of Bath
, Claverton Down, Bath BA2 7AY, United Kingdom
9
Department of Materials, Imperial College London
, Exhibition Road, London SW7 2AZ, United Kingdom
10
Global E3 Institute and Department of Materials Science and Engineering, Yonsei University
, Seoul 03722, South Korea
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Elbert E. M. Chia
Elbert E. M. Chia
b)
1
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University
, Singapore
637371, Singapore
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Daming Zhao
1
Jonathan M. Skelton
2
Hongwei Hu
3
Chan La-o-vorakiat
4,5
Jian-Xin Zhu
6,7
Rudolph A. Marcus
1,8
Maria-Elisabeth Michel-Beyerle
1
Yeng Ming Lam
3
Aron Walsh
2,9,10,a)
Elbert E. M. Chia
1,b)
1
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University
, Singapore
637371, Singapore
2
Department of Chemistry, University of Bath
, Claverton Down, Bath BA2 7AY, United Kingdom
3
School of Materials Science and Engineering, Nanyang Technological University
, Singapore
639798, Singapore
4
Nanoscience and Nanotechnology Graduate Program, King Mongkut's University of Technology Thonburi
, Bangkok 10140, Thailand
5
Theoretical and Computational Science Center (TaCS), Faculty of Science, King Mongkut's University of Technology Thonburi
, Bangkok 10140, Thailand
6
Theoretical Division, Los Alamos National Laboratory
, Los Alamos, New Mexico 87545, USA
7
Center for Integrated Nanotechnologies, Los Alamos National Laboratories
, Los Alamos, New Mexico 87545, USA
8
Noyes Laboratory, California Institute of Technology
, Pasadena, California 91125, USA
9
Department of Materials, Imperial College London
, Exhibition Road, London SW7 2AZ, United Kingdom
10
Global E3 Institute and Department of Materials Science and Engineering, Yonsei University
, Seoul 03722, South Korea
a)
Electronic mail: [email protected]
b)
Electronic mail: [email protected]
Appl. Phys. Lett. 111, 201903 (2017)
Article history
Received:
June 29 2017
Accepted:
November 02 2017
Citation
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; Low-frequency optical phonon modes and carrier mobility in the halide perovskite CH3NH3PbBr3 using terahertz time-domain spectroscopy. Appl. Phys. Lett. 13 November 2017; 111 (20): 201903. https://doi.org/10.1063/1.4993524
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