Ab initio design of enhanced and sign-reversible spin Hall and spin Nernst conductivity in skutterudite materials
Abstract
The search for novel materials capable of robust spin-current generation remains an active area of research. Here, we investigate the intrinsic spin Hall and spin Nernst effects in Co- and Rh-based skutterudites and explore their enhancement through heavy-metal substitution and site-selective doping. Using first-principles calculations and Wannier-based tight-binding models, we analyze the spin Berry curvature and spin-transport responses of pristine MX3, where M = Co, Rh and X = As, Sb, as well as chemically modified systems. Despite sizable momentum-resolved spin Berry curvature, the pristine compounds exhibit relatively small net spin Hall responses due to substantial cancellation across the Brillouin zone. Isoelectronic Ir and Bi substitution at 8c Wycoff M site produces little enhancement near the EF, whereas non-isoelectronic Pt substitution yields a relatively better response. Most interestingly, the incorporation of Pt at the interstitial 2a Wycoff site of RhAs3 nearly doubles the spin Hall conductivity to ∼400 (ℏ/e)(Ω,cm)−1 near the EF when compared to Pt substitution at 8c position. At 300 K, the same interstitially filled system exhibits a spin Nernst conductivity of ∼1.46 (ℏ/e),A,m−1K−1 at the EF, nearly an order of magnitude larger than that of M-site Pt substitution. The enhanced responses arise from Pt 5d states, strong spin-orbit coupling, and avoided crossings that generate pronounced spin-Berry-curvature hot spots. These results demonstrate that site-selective chemical engineering can effectively overcome momentum-space cancellation resulting in enhanced spin Hall and spin Nernst responses in skutterudites. Our results provide a possible route towards robust spin-current generation in this class of materials.
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BibTeX
@misc{debnath2026initio,
title = {{Ab initio design of enhanced and sign-reversible spin Hall and spin Nernst conductivity in skutterudite materials}},
author = {Saikat Debnath and Babu Baijnath Prasad and Shishir Kumar Pandey},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.02998},
eprint = {2610.02998},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.02998},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Ab initio design of enhanced and sign-reversible spin Hall and spin Nernst conductivity in skutterudite materials
AU - Saikat Debnath
AU - Babu Baijnath Prasad
AU - Shishir Kumar Pandey
PY - 2026
DA - 2026/10/02
PB - arXiv
DO - 10.48550/arxiv.2610.02998
UR - https://arxiv.org/abs/2610.02998
AB - The search for novel materials capable of robust spin-current generation remains an active area of research. Here, we investigate the intrinsic spin Hall and spin Nernst effects in Co- and Rh-based skutterudites and explore their enhancement through heavy-metal substitution and site-selective doping. Using first-principles calculations and Wannier-based tight-binding models, we analyze the spin Berry curvature and spin-transport responses of pristine MX_3, where M = Co, Rh and X = As, Sb, as well as chemically modified systems. Despite sizable momentum-resolved spin Berry curvature, the pristine compounds exhibit relatively small net spin Hall responses due to substantial cancellation across the Brillouin zone. Isoelectronic Ir and Bi substitution at 8c Wycoff M site produces little enhancement near the E_F, whereas non-isoelectronic Pt substitution yields a relatively better response. Most interestingly, the incorporation of Pt at the interstitial 2a Wycoff site of RhAs_3 nearly doubles the spin Hall conductivity to ∼400 (ℏ/e)(Ω,cm)^−1 near the E_F when compared to Pt substitution at 8c position. At 300 K, the same interstitially filled system exhibits a spin Nernst conductivity of ∼1.46 (ℏ/e),A,m^−1K^−1 at the E_F, nearly an order of magnitude larger than that of M-site Pt substitution. The enhanced responses arise from Pt 5d states, strong spin-orbit coupling, and avoided crossings that generate pronounced spin-Berry-curvature hot spots. These results demonstrate that site-selective chemical engineering can effectively overcome momentum-space cancellation resulting in enhanced spin Hall and spin Nernst responses in skutterudites. Our results provide a possible route towards robust spin-current generation in this class of materials.
ER -