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, Bin Hu

Research output: Contribution to journalArticlepeer-review

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.

Original languageEnglish
Article number4247
JournalNature Communications
Volume16
Issue number1
DOIs
StatePublished - Dec 2025

Funding

The experimental studies were performed by using the time-resolved magneto-optical instrumentations supported by DURIP funding (FA9550-18-1-0472 Bin Hu) at the Institute of Advanced Materials and Manufacturing at the University of Tennessee. This research used the resources of the Center for Nanophase Materials Sciences (CNMS) under CNMS user program and Neutron Scattering Division (NSD). CNMS and NSD are DOE Office of Science User Facilities. This manuscript has been co-authored (Oak Ridge National Laboratory: Valeria Lauter, Jong Kuem, Haile Ambaye) by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The United States Government retains, and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doepublic-access-plan ).

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