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Title: Detection of Rashba spin splitting in 2D organic-inorganic perovskite via precessional carrier spin relaxation

Abstract

The strong spin-orbit interaction in the organic-inorganic perovskites tied to the incorporation of heavy elements (e.g., Pb and I) makes these materials interesting for applications in spintronics. In conjunction with a lack of inversion symmetry associated with distortions of the metal-halide octahedra, surfaces and interfaces, or the application of a bias, the Rashba effect (used in spin field-effect transistors and spin filters) has been predicted to be much larger in these materials than in traditional III-V semiconductors such as GaAs. Evidence of strong Rashba coupling has been observed in both 3D (bulk) and 2D perovskites, with the relative role of bulk and surface Rashba contributions in the former case under active debate. The varying size of the reported spin splittings points to the need for more experimental studies of Rashba effects in the organic-inorganic perovskite family of materials. Here, we apply time-resolved circular dichroism techniques to the study of carrier spin dynamics in a 2D perovskite thin film [(BA)2MAPb2I7; BA = CH3(CH2)3NH3, MA = CH3NH3]. Our findings confirm the presence of a Rashba spin splitting via the dominance of precessional spin relaxation induced by the Rashba effective magnetic field (also known as D’yakonov Perel spin relaxation). The size of themore » Rashba spin splitting in our system was extracted from simulations of the measured spin dynamics incorporating LO-phonon and electron-electron scattering, yielding a value of 10 meV at an electron energy of 50 meV above the band gap, representing a 20 times larger value than in GaAs quantum wells.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [2];  [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Dalhousie Univ., Halifax, NS (Canada)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Washington State Univ., Pullman, WA (United States)
Publication Date:
Research Org.:
Univ. of California, Santa Barbara, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1611841
Alternate Identifier(s):
OSTI ID: 1567930
Grant/Contract Number:  
SC0012541
Resource Type:
Accepted Manuscript
Journal Name:
APL Materials
Additional Journal Information:
Journal Volume: 7; Journal Issue: 8; Journal ID: ISSN 2166-532X
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Science & Technology - Other Topics; Materials Science; Physics

Citation Formats

Todd, Seth B., Riley, Drew B., Binai-Motlagh, Ali, Clegg, Charlotte, Ramachandran, Ajan, March, Samuel A., Hoffman, Justin M., Hill, Ian G., Stoumpos, Constantinos C., Kanatzidis, Mercouri G., Yu, Zhi-Gang, and Hall, Kimberley C. Detection of Rashba spin splitting in 2D organic-inorganic perovskite via precessional carrier spin relaxation. United States: N. p., 2019. Web. doi:10.1063/1.5099352.
Todd, Seth B., Riley, Drew B., Binai-Motlagh, Ali, Clegg, Charlotte, Ramachandran, Ajan, March, Samuel A., Hoffman, Justin M., Hill, Ian G., Stoumpos, Constantinos C., Kanatzidis, Mercouri G., Yu, Zhi-Gang, & Hall, Kimberley C. Detection of Rashba spin splitting in 2D organic-inorganic perovskite via precessional carrier spin relaxation. United States. https://doi.org/10.1063/1.5099352
Todd, Seth B., Riley, Drew B., Binai-Motlagh, Ali, Clegg, Charlotte, Ramachandran, Ajan, March, Samuel A., Hoffman, Justin M., Hill, Ian G., Stoumpos, Constantinos C., Kanatzidis, Mercouri G., Yu, Zhi-Gang, and Hall, Kimberley C. Fri . "Detection of Rashba spin splitting in 2D organic-inorganic perovskite via precessional carrier spin relaxation". United States. https://doi.org/10.1063/1.5099352. https://www.osti.gov/servlets/purl/1611841.
@article{osti_1611841,
title = {Detection of Rashba spin splitting in 2D organic-inorganic perovskite via precessional carrier spin relaxation},
author = {Todd, Seth B. and Riley, Drew B. and Binai-Motlagh, Ali and Clegg, Charlotte and Ramachandran, Ajan and March, Samuel A. and Hoffman, Justin M. and Hill, Ian G. and Stoumpos, Constantinos C. and Kanatzidis, Mercouri G. and Yu, Zhi-Gang and Hall, Kimberley C.},
abstractNote = {The strong spin-orbit interaction in the organic-inorganic perovskites tied to the incorporation of heavy elements (e.g., Pb and I) makes these materials interesting for applications in spintronics. In conjunction with a lack of inversion symmetry associated with distortions of the metal-halide octahedra, surfaces and interfaces, or the application of a bias, the Rashba effect (used in spin field-effect transistors and spin filters) has been predicted to be much larger in these materials than in traditional III-V semiconductors such as GaAs. Evidence of strong Rashba coupling has been observed in both 3D (bulk) and 2D perovskites, with the relative role of bulk and surface Rashba contributions in the former case under active debate. The varying size of the reported spin splittings points to the need for more experimental studies of Rashba effects in the organic-inorganic perovskite family of materials. Here, we apply time-resolved circular dichroism techniques to the study of carrier spin dynamics in a 2D perovskite thin film [(BA)2MAPb2I7; BA = CH3(CH2)3NH3, MA = CH3NH3]. Our findings confirm the presence of a Rashba spin splitting via the dominance of precessional spin relaxation induced by the Rashba effective magnetic field (also known as D’yakonov Perel spin relaxation). The size of the Rashba spin splitting in our system was extracted from simulations of the measured spin dynamics incorporating LO-phonon and electron-electron scattering, yielding a value of 10 meV at an electron energy of 50 meV above the band gap, representing a 20 times larger value than in GaAs quantum wells.},
doi = {10.1063/1.5099352},
journal = {APL Materials},
number = 8,
volume = 7,
place = {United States},
year = {Fri Aug 16 00:00:00 EDT 2019},
month = {Fri Aug 16 00:00:00 EDT 2019}
}

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Works referencing / citing this record:

Ultrafast acoustic phonon scattering in CH 3 NH 3 PbI 3 revealed by femtosecond four-wave mixing
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Resonant free-carrier absorption in 2D hybrid organic-inorganic perovskites: The Rashba effect or small polarons?
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