Spin-dependent interactions in orbital-density-dependent functionals: non-collinear Koopmans spectral functionals
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arXiv
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| Format: | Preprint |
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2024
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| _version_ | 1866916332336840704 |
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| author | Marrazzo, Antimo Colonna, Nicola |
| author_facet | Marrazzo, Antimo Colonna, Nicola |
| contents | The presence of spin-orbit coupling or non-collinear magnetic spin states can have dramatic effects on the ground-state and spectral properties of materials, in particular on the band structure. Here, we develop non-collinear Koopmans-compliant functionals based on Wannier functions and density-functional perturbation theory, targeting accurate spectral properties in the quasiparticle approximation. Our non-collinear Koopmans-compliant theory involves functionals of four-component orbitals densities, that can be obtained from the charge and spin-vector densities of Wannier functions. We validate our approach on four emblematic non-magnetic and magnetic semiconductors where the effect of spin-orbit coupling goes from small to very large: the III-IV semiconductor GaAs, the transition-metal dichalcogenide WSe$_2$, the cubic perovskite CsPbBr$_3$, and the ferromagnetic semiconductor CrI$_3$. The predicted band gaps are comparable in accuracy to state-of-the-art many-body perturbation theory and include spin-dependent interactions and screening effects that are missing in standard diagrammatic approaches based on the random phase approximation. While the inclusion of orbital- and spin-dependent interactions in many-body perturbation theory requires self-screening or vertex corrections, they emerge naturally in the Koopmans-functionals framework. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2402_14575 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Spin-dependent interactions in orbital-density-dependent functionals: non-collinear Koopmans spectral functionals Marrazzo, Antimo Colonna, Nicola Materials Science The presence of spin-orbit coupling or non-collinear magnetic spin states can have dramatic effects on the ground-state and spectral properties of materials, in particular on the band structure. Here, we develop non-collinear Koopmans-compliant functionals based on Wannier functions and density-functional perturbation theory, targeting accurate spectral properties in the quasiparticle approximation. Our non-collinear Koopmans-compliant theory involves functionals of four-component orbitals densities, that can be obtained from the charge and spin-vector densities of Wannier functions. We validate our approach on four emblematic non-magnetic and magnetic semiconductors where the effect of spin-orbit coupling goes from small to very large: the III-IV semiconductor GaAs, the transition-metal dichalcogenide WSe$_2$, the cubic perovskite CsPbBr$_3$, and the ferromagnetic semiconductor CrI$_3$. The predicted band gaps are comparable in accuracy to state-of-the-art many-body perturbation theory and include spin-dependent interactions and screening effects that are missing in standard diagrammatic approaches based on the random phase approximation. While the inclusion of orbital- and spin-dependent interactions in many-body perturbation theory requires self-screening or vertex corrections, they emerge naturally in the Koopmans-functionals framework. |
| title | Spin-dependent interactions in orbital-density-dependent functionals: non-collinear Koopmans spectral functionals |
| topic | Materials Science |
| url | https://arxiv.org/abs/2402.14575 |