Emergence of insulating ferro- and ferrimagnetism with enhanced optical properties in double-double perovskite oxides
Phys. Rev. B 112, 104423 – Published 15 September, 2025
DOI: https://doi.org/10.1103/fq9d-223r
Abstract
The emergence of ferro- and ferrimagnetic behavior in insulating materials is uncommon, largely due to Hund's rules. Utilizing symmetry analysis, first-principles methods, and classical Monte Carlo simulations, we report technologically important insulating ferro- and ferrimagnetic double-double perovskite oxides. Our study predicts (, Cr, Mn, Co, and Ni) as promising candidates for spintronic and optical applications exhibiting band gaps between 1.3 and 1.9 eV. We explain the mechanisms driving band-gap openings and magnetic exchange interactions in these ferro- and ferrimagnetic compounds. Monte Carlo simulations together with state-of-the-art orbital-decomposed exchange parameter analysis reveal intriguing variations in magnetic transition temperatures (up to 242 K) and the corresponding exchange mechanisms in all compounds. In addition, we assess the thermodynamic and dynamic stability of these compounds to comment on the feasibility of these systems.