Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals
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Type
ArticleAuthors
Frohna, KyleDeshpande, Tejas
Harter, John
Peng, Wei
Barker, Bradford A.
Neaton, Jeffrey B.
Louie, Steven G.
Bakr, Osman
Hsieh, David
Bernardi, Marco
KAUST Department
Physical Sciences and Engineering (PSE) DivisionMaterials Science and Engineering Program
KAUST Catalysis Center (KCC)
Date
2018-05-02Metadata
Show full item recordAbstract
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.Citation
Frohna K, Deshpande T, Harter J, Peng W, Barker BA, et al. (2018) Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals. Nature Communications 9. Available: http://dx.doi.org/10.1038/s41467-018-04212-w.Sponsors
M.B. acknowledges partial support from start-up funds and from the Space Solar Program Initiative at the California Institute of Technology. K.F. thanks the California Institute of Technology for support through the SURF fellowship program, and Peter Foley and Linn Leppert for fruitful discussions. SHG-RA measurements were supported by the U. S. Department of Energy under grant DE-SC0010533. D.H. also acknowledges funding for instrumentation from the Institute for Quantum Information and Matter, an NSF Physics Frontiers Center (PHY-1125565) with support of the Gordon and Betty Moore Foundation through grant GBMF1250. O.M.B and W.P. acknowledge the support of KAUST. J.B.N. and S.G.L. were supported by the U.S. Department of Energy, Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05CH11231, through the Theory FWP (KC2301) at Lawrence Berkeley National Laboratory (LBNL). This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02- 05CH11231.Publisher
Springer NatureJournal
Nature CommunicationsISSN
2041-1723PubMed ID
29739939Handle URI
http://hdl.handle.net/10754/627901Additional Links
https://www.nature.com/articles/s41467-018-04212-wScopus Count
Except where otherwise noted, this item's license is described as The final publication is available at Springer via http://dx.doi.org/10.1038/s41467-018-04212-w