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

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.

doi:10.1002/adom.202101232

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

Journal Article · Mon Oct 18 00:00:00 EDT 2021 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.202101232· OSTI ID:1976228

^[1]; Amerling, Eric ^[2]; Ngo, Tu Anh ^[3]; Luong, Hoang M. ^[3]; Hansen, Kameron ^[2]; Pham, Huy T. ^[4]; Vu, Tuoc N. ^[5]; Tran, Huan ^[6]; Whittaker‐Brooks, Luisa ^[2]; ^[3]

University of Georgia, Athens, GA (United States); OSTI
University of Utah, Salt Lake City, UT (United States)
University of Georgia, Athens, GA (United States)
University Ha Dong, Hanoi (Vietnam)
Hanoi University of Science and Technology, Hanoi (Vietnam)
Georgia Institute of Technology, Atlanta, GA (United States)

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). In this report 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-1Pb_nI_3n+1 (where MA = CH₃NH₃ and BA = CH₃(CH₂)₃NH₃). 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 [PbI₆]^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.

View Accepted Manuscript (DOE)

Research Organization:: University of Georgia, Athens, GA (United States); University of Utah, Salt Lake City, UT (United States)

Sponsoring Organization:: Stylenquaza LLC.DBA Vicostone USA; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); Vingroup Innovation Foundation (VINIF)

Grant/Contract Number:: SC0019041

OSTI ID:: 1976228

Alternate ID(s):: OSTI ID: 1826805

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 1 Vol. 10; ISSN 2195-1071

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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