Abstract
Controlling the flow of angular momentum in solids is central to next-generation electronic technologies, particularly in spintronics and the emerging field of orbitronics, where the orbital motion of electrons plays an active role. However, predicting how these quantities behave in realistic materials with surfaces, interfaces, and disorder remains a major theoretical challenge. To address this problem, we develop a real-space first-principles method based on density functional theory to investigate orbitronic phenomena in transition metals. Using the Real-Space Linear Muffin-Tin Orbital method within the Atomic Sphere Approximation (RS-LMTO-ASA) combined with a Chebyshev polynomial expansion of the Green’s functions, we compute orbital (spin) Hall transport and orbital (spin) accumulation directly in real space. The approach scales linearly with the number of nonequivalent atoms in the unit cell and naturally incorporates disorder, finite-size effects, and interface roughness. We apply the method to a wide range of transition-metal systems, computing bulk orbital and spin Hall conductivities, layer-resolved accumulations in finite slabs, and the corresponding responses in FM/TM bilayers. Our results capture both nonmagnetic and magnetic cases, demonstrating how surface and interfacial electronic structure, as well as broken time-reversal symmetry, modify the relation between bulk conductivities and local accumulations. Our methodology provides a scalable and flexible approach for realistic simulations of orbital transport phenomena in complex heterostructures.
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The data supporting the findings of this study are available from the corresponding authors upon request.
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Acknowledgements
R.C. acknowledges insightful discussions with Danny Thonig and Roberto Bechara Muniz. T.G.R. acknowledges support from the EIC Pathfinder OPEN grant 101129641 “OBELIX”, the Brazilian agency CNPq and insightful discussions with Dongwook Go. H.U.R.S. acknowledges financial support from the Swedish Research Council (Vetenskapsra˙det, VR) grant number 2024-04652 and funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement No. 854843-FASTCORR). A.B. acknowledges support from eSSENCE, the Carl Trygger Foundation and the AI4Research center at Uppsala University. A.B.K. acknowledges support from CAPES and CNPq, Brazil; the INCT of Materials Informatics and the INCT of Spintronics and Advanced Magnetic Nanostructures, CNPq, Brazil.
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T.G.R. developed the linear-response formalism using a Chebyshev expansion. H.U.R.S. and R.C. were responsible for implementing the formalism within the RS-LMTO-ASA framework. R.C., T.G.R., H.U.R.S., A.B. and A.B.K. contributed equally to the discussion of the results and to the preparation of the manuscript.
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Cardias, R., Strand, H.U.R., Bergman, A. et al. Real-space first-principles approach to orbitronic phenomena in metallic multilayers. Commun Phys (2026). https://doi.org/10.1038/s42005-026-02609-4
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DOI: https://doi.org/10.1038/s42005-026-02609-4
