Publication date: 22nd July 2026
Hybrid organic–inorganic metal halide perovskites (HOIPs) have attracted significant attention due to their structural and chemical versatility that offers an ideal platform to engineer not only their optoelectronic behavior [1], but also their magnetic characteristics, making them promising candidates for spintronic applications [2-5]. Hybrid double perovskites and magnetic doped halide perovskites have provided an additional way to tune the properties of HOIPs [6-8]. Through the combination of trivalent metal cations, such as In3+/Ru3+/Fe3+/Mo3+, with monovalent cation M+, researchers have been able to tune the magnetism in hybrid metal halides. However, the influence of isovalent metal cations with unpaired spins has been scarcely investigated [9]. In this work, we studied three different doped compounds, (PEA)2M11−xM2xCl4 (M = Cu2+, Mn2+, Co2+; PEA = phenethylammonium). In each system we explore the incorporation of two different metallic cations with different spin-configuration in order to study the effect of the dopant on the final magnetic and optical properties of the material. The compounds have been synthetized by common chemical approaches and optimized protocols led to single-phase crystals for low dopant amount (x < 0.1). Optically, all the doped systems changed in color and band-gap when compared to the undoped compound, which also has an additional effect on the photoluminescence emission of Mn2+ based HOIPs. In terms of magnetic properties, although the antiferromagnetic behavior in (PEA)2Mn1−xCoxCl4 is kept for all the compositions studied, the doping promotes changes in the Neel temperature from 45 K to 62 K and even the disappearance of magnetic phenomena, such as spin flop and spin canting. On the opposite, doping has negligible effects on (PEA)2Mn1−xCuxCl4 system, which behaves as canted antiferromagnet, and (PEA)2Cu1−xCoxCl4, which presents ferromagnetic properties. Therefore, our work proves that transition metal doping is a promising strategy to modify the optical and magnetic properties of layered HOIPs, providing an approach to create tailored 2D magnets for future spintronic applications. Furthermore, our results emphasize the importance of the proper selection of the host crystal and guest dopant to alter the 2D magnetism [10].
The authors acknowledge funding from MICIU/AEI/10.13039/501100011033 (Grant CEX2020-001038M); from MICIU/AEI and ERDF/EU (Projects PID2021-122511OBI00, PID2021-128004NB-C21, PID2024-157558NB-C21, PID2024-157558NB-C22, and PID2024-155708OB-I00); from MICIU/AEI and European Union NextGenerationEU/PRTR (Project PCI2021-122038-2A). B.M.-G. and M.G. gratefully acknowledge support from MICIU/AEI and the European Union NextGenerationEU/PRTR (grant nos. RYC2021-034836-I and RYC2021-031705-I, respectively). S.M. acknowledges support from the Department of Education of the Basque Government under the Predoctoral Programme for the Training of Nondoctoral Research Staff. Y.A. and L.O.-V. are thankful for the funding from Spanish MICIU/AEI/10.13039/501100011033 and ESF+ (PhD grants PRE2021-099999 and PRE2022-104385, respectively). A.M.-A. acknowledges support from the Basque Science Foundation for Science (IKERBASQUE), POLYMAT, the University of the Basque Country, Diputación de Guipúzcoa, Gobierno Vasco (PIBA_2024_1_0030 and BERC programme), Agencia Estatal de Investigación (Projects PID2021-124484OB-I00, PID2024-157565NB-I00, PCI2022-132921, CEX2020-001067-M and María de Maeztu Excellence Unit CEX2023-001303-M funded by MCIN/AEI/10.13039/501100011033and European Union NextGenerationEU/PRTR).
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