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Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites.

  • Author(s): Wu, Xiaoxi
  • Tan, Liang Z
  • Shen, Xiaozhe
  • Hu, Te
  • Miyata, Kiyoshi
  • Trinh, M Tuan
  • Li, Renkai
  • Coffee, Ryan
  • Liu, Shi
  • Egger, David A
  • Makasyuk, Igor
  • Zheng, Qiang
  • Fry, Alan
  • Robinson, Joseph S
  • Smith, Matthew D
  • Guzelturk, Burak
  • Karunadasa, Hemamala I
  • Wang, Xijie
  • Zhu, Xiaoyang
  • Kronik, Leeor
  • Rappe, Andrew M
  • Lindenberg, Aaron M
  • et al.
Abstract

Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.

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