Magnetism in a 2D Hybrid Ruddlesden-Popper Perovskite through Charge Redistribution Driven by an Organic Functional Spacer

J Phys Chem Lett. 2022 Feb 17;13(6):1406-1415. doi: 10.1021/acs.jpclett.1c04216. Epub 2022 Feb 4.

Abstract

Two-dimensional Ruddlesden-Popper (RP) perovskites are emerging materials offering great synthetic versatility and remarkable features due to the tunability of their crystal structure. We present a novel strategy to provide magnetism in a 2D RP perovskite using histidine molecules as a spacer, which could induce charge rebalancing at the interface of the inorganic layer. We observe that the amide and imidazole groups are close to Pb ions. The interaction with the imidazole indicates that this functional group, possibly assisted by the carboxyl close to the vicinity of the amine terminal, is inducing charge rearrangement from Pb2+ to paramagnetic Pb3+ ions, resulting in a positive magnetic moment. This magnetized 2D hybrid perovskites can be classified as a novel class of promising materials showing a magnetic moment at their interface, which may result in intriguing physical properties due to a delicate balance between magnetism and a quantum well confinement effect in the inorganic layer.