Origin of Dopant-Carrier Exchange Coupling and Excitonic Zeeman Splitting in Mn<sup>2+</sup>-Doped Lead Halide Perovskite Nanocrystals
I-Hsuan Yeh, Mahdieh Ghobadifard, Feng Lin, Victor A. Galievsky, Pavle V. Radovanovic
Abstract
Low-dimensional metal halide perovskites have unique optical and electrical properties that render them attractive for the design of diluted magnetic semiconductors. However, the nature of dopant-exciton exchange interactions that result in spin-polarization of host-lattice charge carriers as a basis for spintronics remains unexplored. Here, we investigate Mn 2+ -doped CsPbCl 3 nanocrystals using magnetic circular dichroism spectroscopy and show that Mn 2+ dopants induce excitonic Zeeman splitting which is strongly dependent on the nature of the band-edge structure. We demonstrate that the largest splitting corresponds to exchange interactions involving the excited state at the M-point along the spin–orbit split-off conduction band edge. This splitting gives rise to an absorption-like C -term excitonic MCD signal, with the estimated effective g -factor ( g eff ) of ca. 70. The results of this work help resolve the assignment of absorption transitions observed for metal halide perovskite nanocrystals and allow for a design of new diluted magnetic semiconductor materials for spintronics applications.