Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional
Abstract Accurate prediction of electronic and optical excitations in van der Waals (vdW) materials is a long-standing challenge for density functional theory. The recent Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has proven successful in non-empirical de...
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| Format: | Article |
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Nature Portfolio
2024-12-01
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| Series: | npj Computational Materials |
| Online Access: | https://doi.org/10.1038/s41524-024-01478-1 |
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| author | María Camarasa-Gómez Stephen E. Gant Guy Ohad Jeffrey B. Neaton Ashwin Ramasubramaniam Leeor Kronik |
| author_facet | María Camarasa-Gómez Stephen E. Gant Guy Ohad Jeffrey B. Neaton Ashwin Ramasubramaniam Leeor Kronik |
| author_sort | María Camarasa-Gómez |
| collection | DOAJ |
| description | Abstract Accurate prediction of electronic and optical excitations in van der Waals (vdW) materials is a long-standing challenge for density functional theory. The recent Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has proven successful in non-empirical determination of electronic band gaps and optical absorption spectra for covalent and ionic crystals. However, for vdW materials the tuning of the material- and structure-dependent functional parameters has only been attained semi-empirically. Here, we present a non-empirical WOT-SRSH approach applicable to vdW materials, with the optimal functional parameters transferable between monolayer and bulk. We apply this methodology to prototypical vdW materials: black phosphorus, molybdenum disulfide, and hexagonal boron nitride (in the latter case including zero-point renormalization). We show that the WOT-SRSH approach consistently achieves accuracy levels comparable to experiments and many-body perturbation theory (MBPT) calculations for band structures and optical absorption spectra, both on its own and as an optimal starting point for MBPT calculations. |
| format | Article |
| id | doaj-art-c266285a3d704646a8885fd2b8f6161f |
| institution | DOAJ |
| issn | 2057-3960 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Computational Materials |
| spelling | doaj-art-c266285a3d704646a8885fd2b8f6161f2025-08-20T02:43:33ZengNature Portfolionpj Computational Materials2057-39602024-12-011011910.1038/s41524-024-01478-1Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functionalMaría Camarasa-Gómez0Stephen E. Gant1Guy Ohad2Jeffrey B. Neaton3Ashwin Ramasubramaniam4Leeor Kronik5Department of Molecular Chemistry and Materials Science, Weizmann Institute of ScienceDepartment of Physics, University of CaliforniaDepartment of Molecular Chemistry and Materials Science, Weizmann Institute of ScienceDepartment of Physics, University of CaliforniaDepartment of Mechanical and Industrial Engineering, University of Massachusetts AmherstDepartment of Molecular Chemistry and Materials Science, Weizmann Institute of ScienceAbstract Accurate prediction of electronic and optical excitations in van der Waals (vdW) materials is a long-standing challenge for density functional theory. The recent Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has proven successful in non-empirical determination of electronic band gaps and optical absorption spectra for covalent and ionic crystals. However, for vdW materials the tuning of the material- and structure-dependent functional parameters has only been attained semi-empirically. Here, we present a non-empirical WOT-SRSH approach applicable to vdW materials, with the optimal functional parameters transferable between monolayer and bulk. We apply this methodology to prototypical vdW materials: black phosphorus, molybdenum disulfide, and hexagonal boron nitride (in the latter case including zero-point renormalization). We show that the WOT-SRSH approach consistently achieves accuracy levels comparable to experiments and many-body perturbation theory (MBPT) calculations for band structures and optical absorption spectra, both on its own and as an optimal starting point for MBPT calculations.https://doi.org/10.1038/s41524-024-01478-1 |
| spellingShingle | María Camarasa-Gómez Stephen E. Gant Guy Ohad Jeffrey B. Neaton Ashwin Ramasubramaniam Leeor Kronik Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional npj Computational Materials |
| title | Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional |
| title_full | Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional |
| title_fullStr | Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional |
| title_full_unstemmed | Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional |
| title_short | Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional |
| title_sort | excitations in layered materials from a non empirical wannier localized optimally tuned screened range separated hybrid functional |
| url | https://doi.org/10.1038/s41524-024-01478-1 |
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