Publication date: 21st July 2025
The discussed work deals with the control and characterization of spin degrees of freedom of photo-generated carriers in halide perovskite materials via magnetic doping. The materials under consideration, CsPbBr3 and PEA2PbI4, include the diluted concentration of Ni2+ or Mn2+ ions at a metal substitution position. Magnetic doping was implemented extensively in colloidal quantum dots, but with a limited way in the perovskite semiconductors, wherein the latter possesses other significant properties (e.g., dopant-carrier spin-exchange interactions, a large g-factor and extension of spin relaxation time).
Our work reports a thorough investigation of spin degrees of freedom in the mentioned materials, monitored by magneto-photoluminescence and optically detected magnetic resonance (ODMR) spectroscopies, which provide a significant information on exact location of host carriers and dopants, as well as examine interactions between them.
specifically, one project focused on a thorough investigation of the influence of Ni2+ dopants on the optical and magneto-optical properties of CsPbBr3 nano-cubes. The study implemented methodologies that are applied to halide perovskites for the first time, like steady-state and transient optically detected magnetic resonance (ODMR) spectroscopy, leading to significant advances that address long-standing debates in this field: (a) A direct identification of defect centers, in conflict with the widely assumed defect-free behavior of halide perovskites; (b) Direct observation of spin-exchange interactions between dopant unpaired electrons and photo-generated carriers, which has not been resolved previously. The extracted physical parameters from the ODMR experiments included: g-factors and their anisotropy, spin exchange interactions, angular momentum, carrier-dopant coupling constants, radiative and spin-lattice relaxation times. A second project focused on the influence of Mn2+ dopants in 2D MA2PbI4 and PEA2PbI4 single crystals, implementing the mentioned magneto-optically spectroscopies, focusing on the added values of the dopant to the so-called Rashba effect (an ongoing project).
The spin properties mentioned here undoubtedly can play an important role in the development of new spin-based technologies.
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