Magnetic proximity effect on excitonic spin states in Mn-doped layered hybrid perovskites

TL;DR

This study demonstrates magnetic proximity effects in Mn-doped layered hybrid perovskites, enabling control over excitonic spin states through magnetic interactions, with potential applications in quantum technologies.

Contribution

First demonstration of polarization control in magnetically doped hybrid perovskites via magnetic proximity effects, linking magnetic moments with exciton spins.

Findings

Circularly polarized photoluminescence correlates with magnetization.

Saturation polarization of 15% at 4 K and 6 T.

Coupling between Mn magnetic moments and exciton spins confirmed.

Abstract

Materials combining the optoelectronic functionalities of semiconductors with control of the spin degree of freedom are highly sought after for the advancement of quantum technology devices. Here, we report the paramagnetic Ruddlesden-Popper hybrid perovskite Mn:(PEA)2PbI4 (PEA = phenethylammonium) in which the interaction of isolated Mn2+ ions with magnetically brightened excitons leads to circularly polarized photoluminescence. Using a combination of superconducting quantum interference device (SQUID) magnetometry and magneto-optical experiments, we find that the Brillouin-shaped polarization curve of the photoluminescence follows the magnetization of the material. This indicates coupling between localized manganese magnetic moments and exciton spins via a magnetic proximity effect. The saturation polarization of 15% at 4 K and 6 T indicates a highly imbalanced spin population and demonstrates that manganese doping enables efficient control of excitonic spin states in Ruddlesden-Popper perovskites. Our finding constitutes the first example of polarization control in magnetically doped hybrid perovskites and will stimulate research on this highly tuneable material platform that promises tailored interactions between magnetic moments and electronic states.