4.3 Article

Elucidating the atomistic origin of anharmonicity in tetragonal CH3NH3PbI3 with Raman scattering

Journal

PHYSICAL REVIEW MATERIALS
Volume 4, Issue 9, Pages -

Publisher

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevMaterials.4.092401

Keywords

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Funding

  1. FGS-WIS
  2. ISF [1861/17]
  3. BSF [2016650]
  4. ERC [850041-ANHARMONIC]
  5. Benoziyo Endowment Fund
  6. Ilse Katz Institute
  7. Henry Chanoch Krenter Institute
  8. Soref New Scientists Start up Fund
  9. Carolito Stiftung
  10. Abraham and Sonia Rochlin Foundation
  11. E. A. Drake and R. Drake, and the Perlman Family
  12. U.S. National Science Foundation [DMR-1719353]
  13. VIEST Fellowship at the University of Pennsylvania
  14. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-FG02-07ER46431]
  15. Division Of Computer and Network Systems
  16. Direct For Computer & Info Scie & Enginr [2016650] Funding Source: National Science Foundation

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Halide perovskite (HP) semiconductors exhibit unique strong coupling between the electronic and structural dynamics. We use Raman polarization-orientation (PO) measurements and ab initio molecular dynamics (AIMD) to investigate the origin and temperature evolution of the strong structural anharmonicity throughout the tetragonal phase of CH3NH3PbI3. Raman PO measurements reveal a soft modelike spectral feature. This mode shows an unusual continuous increase in damping with temperature which is indicative of an anharmonic potential surface. The analysis of AIMD trajectories identifies two major sources of anharmonicity: the orientational unlocking of the [CH3NH3](+) ions and large-amplitude octahedral tilting that continuously increases with temperature. Our work suggests that the standard phonon picture cannot describe the structural dynamics of tetragonal CH3NH3PbI3.

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