Intrinsic Ferromagnetic Semiconductors with High Saturation Magnetization from Hybrid Perovskites

Ferromagnetic semiconductors (FMS) enable simultaneous control of both charge and spin transport of charge carriers, and they have emerged as a class of highly desirable but rare materials for applications in spin field-effect transistors and quantum computing. Organic-inorganic hybrid perovskites with high compositional adjustability and structural versatility can offer unique benefits in the design of FMS but has not been fully explored. Here, a series of molecular FMSs based on the 2D organic-inorganic hybrid perovskite structure, namely (2ampy)CuCl₄ , (3ampy)CuCl₄ , and (4ampy)CuCl₄ , is demonstrated, which exhibits high saturation magnetization, dramatic temperature-dependent conductivity change, and tunable ferromagnetic resonance. Magnetic measurements reveal a high saturation magnetization up to 18.56 emu g^-1 for (4ampy)CuCl₄ , which is one of the highest value among reported hybrid FMSs to date. Conductivity studies of the three FMSs demonstrate that the smaller adjacent octahedron distance in the 2D layer results in higher conductivity. Systematic ferromagnetic resonance investigation shows that the gyromagnetic ratio and Landau factor values are strongly dependent on the types of organic cations used. This work demonstrates that 2D hybrid perovskite materials can simultaneously possess both tunable long-range ferromagnetic ordering and semiconductivity, providing a straightforward strategy for designing and synthesizing high-performance intrinsic FMSs.