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Polar rotor scattering as atomic-level origin of low mobility and thermal conductivity of perovskite CH3NH3PbI3

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  • Bing Li

    (Neutron Science Section, Japan Proton Accelerator Research Complex, Japan Atomic Energy Agency)

  • Yukinobu Kawakita

    (Neutron Science Section, Japan Proton Accelerator Research Complex, Japan Atomic Energy Agency)

  • Yucheng Liu

    (Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education, Institute for Advanced Energy Materials, School of Materials Science and Engineering, Shaanxi Normal University)

  • Mingchao Wang

    (Materials Science and Engineering Program, FAMU-FSU College of Engineering, Florida State University)

  • Masato Matsuura

    (Neutron Science and Technology Center, Comprehensive Research Organization for Science and Society)

  • Kaoru Shibata

    (Neutron Science Section, Japan Proton Accelerator Research Complex, Japan Atomic Energy Agency)

  • Seiko Ohira-Kawamura

    (Neutron Science Section, Japan Proton Accelerator Research Complex, Japan Atomic Energy Agency)

  • Takeshi Yamada

    (Neutron Science and Technology Center, Comprehensive Research Organization for Science and Society)

  • Shangchao Lin

    (Materials Science and Engineering Program, FAMU-FSU College of Engineering, Florida State University)

  • Kenji Nakajima

    (Neutron Science Section, Japan Proton Accelerator Research Complex, Japan Atomic Energy Agency)

  • Shengzhong (Frank) Liu

    (Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education, Institute for Advanced Energy Materials, School of Materials Science and Engineering, Shaanxi Normal University
    Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences)

Abstract

Perovskite CH3NH3PbI3 exhibits outstanding photovoltaic performances, but the understanding of the atomic motions remains inadequate even though they take a fundamental role in transport properties. Here, we present a complete atomic dynamic picture consisting of molecular jumping rotational modes and phonons, which is established by carrying out high-resolution time-of-flight quasi-elastic and inelastic neutron scattering measurements in a wide energy window ranging from 0.0036 to 54 meV on a large single crystal sample, respectively. The ultrafast orientational disorder of molecular dipoles, activated at ∼165 K, acts as an additional scattering source for optical phonons as well as for charge carriers. It is revealed that acoustic phonons dominate the thermal transport, rather than optical phonons due to sub-picosecond lifetimes. These microscopic insights provide a solid standing point, on which perovskite solar cells can be understood more accurately and their performances are perhaps further optimized.

Suggested Citation

  • Bing Li & Yukinobu Kawakita & Yucheng Liu & Mingchao Wang & Masato Matsuura & Kaoru Shibata & Seiko Ohira-Kawamura & Takeshi Yamada & Shangchao Lin & Kenji Nakajima & Shengzhong (Frank) Liu, 2017. "Polar rotor scattering as atomic-level origin of low mobility and thermal conductivity of perovskite CH3NH3PbI3," Nature Communications, Nature, vol. 8(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms16086
    DOI: 10.1038/ncomms16086
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    Cited by:

    1. Paribesh Acharyya & Tanmoy Ghosh & Koushik Pal & Kewal Singh Rana & Moinak Dutta & Diptikanta Swain & Martin Etter & Ajay Soni & Umesh V. Waghmare & Kanishka Biswas, 2022. "Glassy thermal conductivity in Cs3Bi2I6Cl3 single crystal," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Qingyong Ren & Ji Qi & Dehong Yu & Zhe Zhang & Ruiqi Song & Wenli Song & Bao Yuan & Tianhao Wang & Weijun Ren & Zhidong Zhang & Xin Tong & Bing Li, 2022. "Ultrasensitive barocaloric material for room-temperature solid-state refrigeration," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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