Journal
PHYSICAL REVIEW MATERIALS
Volume 4, Issue 5, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevMaterials.4.051601
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Funding
- NSF-BSF program, under NSF [DMR-1719353]
- NSF-BSF program, BSF [2016650]
- FGS-WIS
- ISF [1861/17]
- BSF [2016650]
- ERC [850041-ANHARMONIC]
- Benoziyo Endowment Fund
- Ilse Katz Institute
- Henry Chanoch Krenter Institute
- Soref New Scientists Start up Fund
- Carolito Stiftung
- Abraham AMP
- Sonia Rochlin Foundation
- US NSF [DMR-1719353]
- VIEST Fellowship at the University of Pennsylvania
- Office of Naval Research [N00014-17-1-2574]
- Direct For Computer & Info Scie & Enginr
- Division Of Computer and Network Systems [2016650] Funding Source: National Science Foundation
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In the last decade, hybrid organic-inorganic halide perovskites have emerged as a new type of semiconductor for photovoltaics and other optoelectronic applications. Unlike standard, tetrahedrally bonded semiconductors (e.g., Si and GaAs), the ionic thermal fluctuations in the halide perovskites (i.e., structural dynamics) are strongly coupled to the electronic dynamics. Therefore, it is crucial to obtain accurate and detailed knowledge about the nature of the atomic motions within the crystal. This has proved to be challenging due to low thermal stability and the complex, temperature-dependent structural phase sequence of the halide perovskites. Here, these challenges are overcome and a detailed analysis of the low-frequency lattice mode symmetries is provided in the low-temperature orthorhombic phase of methylammonium-lead iodide. Raman measurements using linearly and circularly polarized light at 1.16 eV excitation are combined with density functional perturbation theory (DFPT). By performing an iterative analysis of Raman polarization-orientation dependence and DFPT mode analysis, the crystal orientation is determined. Subsequently, accounting for birefringence effects detected using circularly polarized light excitation, the symmetries of all of the observed Raman-active modes at 10 K are assigned.
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