Publication date: 22nd July 2026
The development of new technologies has always been accompanied by access to functional materials with targeted, exceptional properties. Looking towards the future, layered hybrid organic-inorganic metal halide perovskites (HOIPs) are poised to play a significant role in optoelectronic, spintronic, and quantum technologies due to their tunable bandgap, high carrier mobility, strong spin-orbit coupling and magnetic ordering.[1-4] However, for their successful integration into devices and development of new applications, understanding the relationship between composition, crystal structure, and optical and magnetic properties, as well as how to control them, is key. Indeed, HOIPs incorporating transition metals are an ideal platform for tuning magnetic (spins) and even optical (photons) due to their chemical and structural versatility.[1,5–8] In this work, we explore the effects of magnetism in the photoluminescence (PL) emission originating from spin-forbidden d-d transitions[7,8] of antiferromagnetic Mn2+ HOIPs with different crystal lattice parameters. Using temperature-dependent PL and PL excitation (PLE) spectroscopy, we demonstrate the complexity of the magneto-optical coupling in these materials and provide new insights into this field. We reveal significant changes in the PL/PLE trends prior to reach long-range magnetic order. Our results highlight the interplay among the magnetic polarons, intrinsic magnetism and crystal structure as the origin of these changes, providing new insights into spin-optoelectronics.[9]
This work was supported under Projects PID2021-122511OB-I00, PID2021-128004NB-C21, PID2024-157558NB-C21, PID2024-157558NB-C22, and PID2024-155708OB-I00 and under the María de Maeztu Units of Excellence Programme (Grant CEX2020-001038-M) funded by Spanish MICIU/AEI/10.13039/501100011033 and by ERDF/EU; Spanish MICIU/AEI/10.13039/501100011033 and ESF+ for Y.A. PhD grant PRE2021-099999); Department of Education of the Basque Government under the Pre-doctoral Programme for the Training of Non-doctoral Research Staff for S.M. PhD grant; “Ramón y Cajal” Programme by the Spanish MICIU/AEI/10.13039/501100011033 and European Union NextGenerationEU/PRTR (grant nos. RYC2021-034836-I and RYC2021-031705-I, respectively). This work was also received financial support from the European Union (ERC, 2D-OPTOSPIN, 101076932), the Zernike Institute for Advanced Materials, and the Research Program “Materials for the Quantum Age” (QuMat – registration number 024.005.006), which is part of the Gravitation program financed by the Dutch Ministry of Education, Culture and Science (OCW).
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