Spin switchable optical phenomena in Rashba band structures through intersystem crossing in momentum space in solution-processing 2D-superlattice perovskite film

Bogdan Dryzhakov, Yipeng Tang, Jong Keum, Haile Ambaye, Jinwoo Kim, Tae-Woo Lee, Valeria Lauter () and Bin Hu ()
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Bogdan Dryzhakov: University of Tennessee
Yipeng Tang: University of Tennessee
Jong Keum: Oak Ridge National Laboratory
Haile Ambaye: Oak Ridge National Laboratory
Jinwoo Kim: Seoul National University
Tae-Woo Lee: Seoul National University
Valeria Lauter: Oak Ridge National Laboratory
Bin Hu: University of Tennessee

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Spin-switchable phenomena are a critical element for the development of spintronic and chiroptic devices. Herein we combine a 2D-superlattice perovskite (4,4-DFPD2PbI4) film with a ferromagnetic cobalt (Co) layer to form a multiferroic perovskite/Co interface, and demonstrate spin-switchable circularly polarized luminescence (CPL) between right-handed σ+ and left-handed σ− polarizations. When the ferromagnetic spins of Co at the Co/perovskite interface are altered between positive and negative magnetic field directions, the CPL from the 2D-superlattice perovskite switches from σ+ to σ− polarization. The magnetic field effects present a unique method to confirm that CPL is generated by the circular-orbital momentum of light-emitting excitons within Rashba band structures, eliminating artifacts involving structural birefringence. Our polarized neutron reflectometry measurements confirm a super long-range spin-orbit interaction occurring in the 2D-superlattice perovskite films. The temperature dependence of spin-switchable phenomenon indicates an extraordinarily long orbital polarization lifetime, reaching microseconds at room temperature and milliseconds at 5 K.

Date: 2025
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DOI: 10.1038/s41467-025-57834-2

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