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Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals.


ABSTRACT: Methylammonium lead iodide perovskite (MAPbI3) exhibits long charge carrier lifetimes that are linked to its high efficiency in solar cells. Yet, the mechanisms governing these unusual carrier dynamics are not completely understood. A leading hypothesis-disproved in this work-is that a large, static bulk Rashba effect slows down carrier recombination. Here, using second harmonic generation rotational anisotropy measurements on MAPbI3 crystals, we demonstrate that the bulk structure of tetragonal MAPbI3 is centrosymmetric with I4/mcm space group. Our calculations show that a significant Rashba splitting in the bandstructure requires a non-centrosymmetric lead iodide framework, and that incorrect structural relaxations are responsible for the previously predicted large Rashba effect. The small Rashba splitting allows us to compute effective masses in excellent agreement with experiment. Our findings rule out the presence of a large static Rashba effect in bulk MAPbI3, and our measurements find no evidence of dynamic Rashba effects.

SUBMITTER: Frohna K 

PROVIDER: S-EPMC5940805 | biostudies-other | 2018 May

REPOSITORIES: biostudies-other

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Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals.

Frohna Kyle K   Deshpande Tejas T   Harter John J   Peng Wei W   Barker Bradford A BA   Neaton Jeffrey B JB   Louie Steven G SG   Bakr Osman M OM   Hsieh David D   Bernardi Marco M  

Nature communications 20180508 1


Methylammonium lead iodide perovskite (MAPbI<sub>3</sub>) exhibits long charge carrier lifetimes that are linked to its high efficiency in solar cells. Yet, the mechanisms governing these unusual carrier dynamics are not completely understood. A leading hypothesis-disproved in this work-is that a large, static bulk Rashba effect slows down carrier recombination. Here, using second harmonic generation rotational anisotropy measurements on MAPbI<sub>3</sub> crystals, we demonstrate that the bulk s  ...[more]

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