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    Emergence of insulating ferro- and ferrimagnetism with enhanced optical properties in double-double perovskite oxides

    Monirul Shaikh1,*, Fengyi Zhou2, Sathiyamoorthy Buvaneswaran1, Rajan Gowsalya1, Trilochan Sahoo1, Duo Wang2,†, and Saurabh Ghosh1,‡

    • *Contact author: msk.phe@gmail.com
    • †Contact author: duo.wang@mpu.edu.mo
    • ‡Contact author: saurabhghosh2802@gmail.com

    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 LaA′MnNiO6 (A′=V, 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 LaA′MnNiO6 compounds. In addition, we assess the thermodynamic and dynamic stability of these compounds to comment on the feasibility of these systems.

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