Strain-induced half-metallicity and giant Wiedemann–Franz violation in monolayer NiI2

Abstract

Reversible control of spin-dependent thermoelectricity via mechanical strain provides a platform for next-generation energy harvesting and thermal logic circuits. Using first-principles and Boltzmann transport calculations, we demonstrate that monolayer NiI₂ undergoes a strain-driven semiconductor-to-half-metal transition, enabled by the selective closure of its spin-down band gap while preserving a robust ferromagnetic ground state. Remarkably, this transition is accompanied by a giant, non-monotonic violation of the Wiedemann–Franz law, with the Lorenz number enhanced up to 7.17L₀. This anomaly arises from a strain-sensitive hybridization between Ni-d and I-p orbitals, leading to spin-polarized transport channels and decoupling of heat and charge currents. These properties make NiI₂ a promising candidate for mechanically gated spin-caloritronic devices and thermal logic elements, where reversible control of heat and spin flow is essential. Our findings position NiI₂ as a model system for exploring non-Fermi-liquid transport and for realizing strain-tunable, energy-efficient functionalities in low-dimensional platforms.