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Title: Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies

Two-dimensional (2D) layered hybrid organic-inorganic halide perovskite semiconductors form natural “multiple quantum wells” that have strong spin-orbit coupling due to the heavy elements in their building blocks. This may lead to “Rashba splitting” close to the extrema in the electron bands. We have used a plethora of ultrafast transient, nonlinear optical spectroscopies and theoretical calculations to study the primary (excitons) and long-lived (free carriers) photoexcitations in thin films of 2D perovskite, namely, (C 6H 5C 2H 4NH 3) 2PbI 4. The density functional theory calculation shows the occurrence of Rashba splitting in the plane perpendicular to the 2D barrier. From the electroabsorption spectrum and photoinduced absorption spectra from excitons and free carriers, we obtain a giant Rashba splitting in this compound, with energy splitting of (40 ± 5) meV and Rashba parameter of (1.6 ± 0.1) eV·Å, which are among the highest Rashba splitting size parameters reported so far. In conclusion, this finding shows that 2D hybrid perovskites have great promise for potential applications in spintronics.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [1]
  1. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Physics and Astronomy
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Nanoscale Science and Technology; Univ. of Maryland, College Park, MD (United States). Maryland NanoCenter
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Nanoscale Science and Technology
  4. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Physics and Astronomy; Nanjing Univ. of Science and Technology, Nanjing (China). School of Electronic and Optical Engineering
  5. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Physics and Astronomy; Technion-Israel Inst. of Technology, Haifa (Israel)
Publication Date:
Grant/Contract Number:
SC0014579; DMR 1121252; 598/14; 30915011202
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 7; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
Univ. of Utah, Salt Lake City, UT (United States)
Sponsoring Org:
USDOE Office of Science (SC); National Science Foundation (NSF); Israel Science Foundation (ISF); National Natural Science Foundation of China (NNSFC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
OSTI Identifier:
1425943

Zhai, Yaxin, Baniya, Sangita, Zhang, Chuang, Li, Junwen, Haney, Paul, Sheng, Chuan-Xiang, Ehrenfreund, Eitan, and Vardeny, Zeev Valy. Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies. United States: N. p., Web. doi:10.1126/sciadv.1700704.
Zhai, Yaxin, Baniya, Sangita, Zhang, Chuang, Li, Junwen, Haney, Paul, Sheng, Chuan-Xiang, Ehrenfreund, Eitan, & Vardeny, Zeev Valy. Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies. United States. doi:10.1126/sciadv.1700704.
Zhai, Yaxin, Baniya, Sangita, Zhang, Chuang, Li, Junwen, Haney, Paul, Sheng, Chuan-Xiang, Ehrenfreund, Eitan, and Vardeny, Zeev Valy. 2017. "Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies". United States. doi:10.1126/sciadv.1700704. https://www.osti.gov/servlets/purl/1425943.
@article{osti_1425943,
title = {Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies},
author = {Zhai, Yaxin and Baniya, Sangita and Zhang, Chuang and Li, Junwen and Haney, Paul and Sheng, Chuan-Xiang and Ehrenfreund, Eitan and Vardeny, Zeev Valy},
abstractNote = {Two-dimensional (2D) layered hybrid organic-inorganic halide perovskite semiconductors form natural “multiple quantum wells” that have strong spin-orbit coupling due to the heavy elements in their building blocks. This may lead to “Rashba splitting” close to the extrema in the electron bands. We have used a plethora of ultrafast transient, nonlinear optical spectroscopies and theoretical calculations to study the primary (excitons) and long-lived (free carriers) photoexcitations in thin films of 2D perovskite, namely, (C6H5C2H4NH3)2PbI4. The density functional theory calculation shows the occurrence of Rashba splitting in the plane perpendicular to the 2D barrier. From the electroabsorption spectrum and photoinduced absorption spectra from excitons and free carriers, we obtain a giant Rashba splitting in this compound, with energy splitting of (40 ± 5) meV and Rashba parameter of (1.6 ± 0.1) eV·Å, which are among the highest Rashba splitting size parameters reported so far. In conclusion, this finding shows that 2D hybrid perovskites have great promise for potential applications in spintronics.},
doi = {10.1126/sciadv.1700704},
journal = {Science Advances},
number = 7,
volume = 3,
place = {United States},
year = {2017},
month = {7}
}

Works referenced in this record:

Preparation and characterization of layered lead halide compounds
journal, March 1991
  • Calabrese, J.; Jones, N. L.; Harlow, R. L.
  • Journal of the American Chemical Society, Vol. 113, Issue 6, p. 2328-2330
  • DOI: 10.1021/ja00006a076