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Title: Strong Rashba-Dresselhaus Effect in Nonchiral 2D Ruddlesden-Popper Perovskites

Abstract

Abstract Chirality transfer from organic chiral molecules to lead halides is theorized as the origin of the strong Rashba‐Dresselhaus effect causing large circular dichroism (CD) and circularly polarized luminescence (CPL) in metal halide perovskites (MHPs). Here, a concrete empirical evidence is provided that such strong CD and CPL can occur even in nonchiral 2D Ruddlesden‐Popper perovskites (RPPs) (BA) 2 (MA) n −1 Pb n I 3 n +1 (where MA = CH 3 NH 3 and BA = CH 3 (CH 2 ) 3 NH 3 ). The CD and CPL responses occurring at the excitonic transition of the MHPs are strongest (≈100 mdeg and 4.8%, respectively) when a single lead halide octahedral [PbI 6 ] 4− layer is repeatedly stacked between two nonchiral molecules BA + ( n  = 1). However, they are rapidly quenched as n increases. It is hypothesized that strong Rashba‐Dresselhaus splitting in the 2D RPPs originates the strong CD and CPL signatures. Density functional theory calculations reveal that the large interlayer distortions in the inorganic layers at the organic/inorganic interface give rise to the strong Rashba‐Dresselhaus splitting. A Rashba‐Dresselhaus field of ≈600 and ≈50 mT for n  = 1 and 2, respectively, is estimated bymore » magnetic circular dichroism spectroscopy. The studies may have significant impact on designing 2D RPPs with large Rashba‐Dresselhaus effects at room temperature for spintronic applications.« less

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [2];  [3];  [4];  [5];  [2]; ORCiD logo [1]
  1. University of Georgia, Athens, GA (United States)
  2. University of Utah, Salt Lake City, UT (United States)
  3. University Ha Dong, Hanoi (Vietnam)
  4. Hanoi University of Science and Technology, Hanoi (Vietnam)
  5. Georgia Institute of Technology, Atlanta, GA (United States)
Publication Date:
Research Org.:
Univ. of Utah, Salt Lake City, UT (United States); Univ. of Georgia, Athens, GA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Stylenquaza LLC.DBA Vicostone USA; Vingroup Innovation Foundation (VINIF)
OSTI Identifier:
1976228
Alternate Identifier(s):
OSTI ID: 1826805
Grant/Contract Number:  
SC0019041; AWD00009492; DE‐SC0019041
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Optical Materials
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2195-1071
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 2D Ruddlesden-Popper perovskites; Rashba-Dresselhaus spin orbit coupling; chirality; circular dichroism; circularly polarized luminescence

Citation Formats

Pham, Minh T., Amerling, Eric, Ngo, Tu Anh, Luong, Hoang M., Hansen, Kameron, Pham, Huy T., Vu, Tuoc N., Tran, Huan, Whittaker‐Brooks, Luisa, and Nguyen, Tho D. Strong Rashba-Dresselhaus Effect in Nonchiral 2D Ruddlesden-Popper Perovskites. United States: N. p., 2021. Web. doi:10.1002/adom.202101232.
Pham, Minh T., Amerling, Eric, Ngo, Tu Anh, Luong, Hoang M., Hansen, Kameron, Pham, Huy T., Vu, Tuoc N., Tran, Huan, Whittaker‐Brooks, Luisa, & Nguyen, Tho D. Strong Rashba-Dresselhaus Effect in Nonchiral 2D Ruddlesden-Popper Perovskites. United States. https://doi.org/10.1002/adom.202101232
Pham, Minh T., Amerling, Eric, Ngo, Tu Anh, Luong, Hoang M., Hansen, Kameron, Pham, Huy T., Vu, Tuoc N., Tran, Huan, Whittaker‐Brooks, Luisa, and Nguyen, Tho D. Mon . "Strong Rashba-Dresselhaus Effect in Nonchiral 2D Ruddlesden-Popper Perovskites". United States. https://doi.org/10.1002/adom.202101232. https://www.osti.gov/servlets/purl/1976228.
@article{osti_1976228,
title = {Strong Rashba-Dresselhaus Effect in Nonchiral 2D Ruddlesden-Popper Perovskites},
author = {Pham, Minh T. and Amerling, Eric and Ngo, Tu Anh and Luong, Hoang M. and Hansen, Kameron and Pham, Huy T. and Vu, Tuoc N. and Tran, Huan and Whittaker‐Brooks, Luisa and Nguyen, Tho D.},
abstractNote = {Abstract Chirality transfer from organic chiral molecules to lead halides is theorized as the origin of the strong Rashba‐Dresselhaus effect causing large circular dichroism (CD) and circularly polarized luminescence (CPL) in metal halide perovskites (MHPs). Here, a concrete empirical evidence is provided that such strong CD and CPL can occur even in nonchiral 2D Ruddlesden‐Popper perovskites (RPPs) (BA) 2 (MA) n −1 Pb n I 3 n +1 (where MA = CH 3 NH 3 and BA = CH 3 (CH 2 ) 3 NH 3 ). The CD and CPL responses occurring at the excitonic transition of the MHPs are strongest (≈100 mdeg and 4.8%, respectively) when a single lead halide octahedral [PbI 6 ] 4− layer is repeatedly stacked between two nonchiral molecules BA + ( n  = 1). However, they are rapidly quenched as n increases. It is hypothesized that strong Rashba‐Dresselhaus splitting in the 2D RPPs originates the strong CD and CPL signatures. Density functional theory calculations reveal that the large interlayer distortions in the inorganic layers at the organic/inorganic interface give rise to the strong Rashba‐Dresselhaus splitting. A Rashba‐Dresselhaus field of ≈600 and ≈50 mT for n  = 1 and 2, respectively, is estimated by magnetic circular dichroism spectroscopy. The studies may have significant impact on designing 2D RPPs with large Rashba‐Dresselhaus effects at room temperature for spintronic applications.},
doi = {10.1002/adom.202101232},
journal = {Advanced Optical Materials},
number = 1,
volume = 10,
place = {United States},
year = {Mon Oct 18 00:00:00 EDT 2021},
month = {Mon Oct 18 00:00:00 EDT 2021}
}

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