Journal
SCIENCE ADVANCES
Volume 3, Issue 7, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.1602388
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Funding
- Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division
- DOE BES Scientific User Facilities Division
- SLAC UED/UEM program development fund
- US Department of Energy, Office of Science - Basic Energy Sciences [ER46980]
- Office of Naval Research [N00014-17-1-2574]
- Austrian Science Fund (FWF) [J3608-N20]
- Dana and Yossie Hollander
- Precourt Institute for Energy
- NSF [DGE-114747, ECCS1542152]
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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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