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

Frohna, Kyle; Deshpande, Tejas; Harter, John; Peng, Wei; Barker, Bradford A.; Neaton, Jeffrey B.; Louie, Steven G.; Bakr, Osman M.; Hsieh, David; Bernardi, Marco

doi:10.1038/s41467-018-04212-w

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

Journal Article · Tue May 08 00:00:00 EDT 2018 · Nature Communications

DOI:https://doi.org/10.1038/s41467-018-04212-w· OSTI ID:1460353

^[1];

^[2]; Harter, John ^[2]; Peng, Wei ^[3]; Barker, Bradford A. ^[4]; Neaton, Jeffrey B. ^[4]; Louie, Steven G. ^[4]; Bakr, Osman M. ^[3]; Hsieh, David ^[2]; Bernardi, Marco ^[2]

California Inst. of Technology (CalTech), Pasadena, CA (United States); Trinity College Dublin, Dublin (Ireland)
California Inst. of Technology (CalTech), Pasadena, CA (United States)
King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Saudi Arabia)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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. Here, 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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1460353

Journal Information:: Nature Communications, Vol. 9, Issue 1; Related Information: © 2018 The Author(s).; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 164 works

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