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Polaron-Driven Switching of Octupolar Order in Doped 5d2 Double Perovskite

Dario Fiore Mosca1,2,3, Lorenzo Celiberti1,4, Leonid V. Pourovskii2,3, and Cesare Franchini1,5

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Phys. Rev. Lett. 137, 046504 – Published 22 July, 2026

DOI: https://doi.org/10.1103/r8v5-h8bq

Abstract

We investigate how doping-induced small polarons impact the low-temperature multipolar orders of the 5d2 double perovskite Ba2CaOsO6. By computing intersite exchange interactions between 5d1 localized hole polarons and 5d2 magnetic ions from first principles, we demonstrate the reversal of the dominant octupolar exchange from ferromagnetic to antiferromagnetic. Solving the corresponding effective Hamiltonian, we find this reversal to account for the progressive suppression of the ferro-octupolar order and the reduction of the ordering temperature upon Na doping. These findings clarify previously ambiguous experimental observations and demonstrate that charge doping in the form of small polarons offers a viable route to tuning intersite exchange interactions in spin-orbit-entangled materials, enabling the emergence of novel quantum orders.

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Phys. Rev. Lett. 137, 046504– Published 22 July, 2026
  • Received 3 December 2025
  • Revised 5 June 2026
  • Accepted 15 June 2026
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