article published Katharina Franzke author Wolf Gero Schmidt author 4680000-0002-2717-5076 Uwe Gerstmann author 1710000-0002-4476-223X 15 department 170 department 295 department 790 department 230 department 429 department 27 department 35 department TRR 142: TRR 142 - Maßgeschneiderte nichtlineare Photonik: Von grundlegenden Konzepten zu funktionellen Strukturen project TRR 142 - A: TRR 142 - Project Area A project TRR 142 - B: TRR 142 - Project Area B project TRR 142 - A11: TRR 142 - Subproject A11 project TRR 142 - B07: TRR 142 - Polaronen-Einfluss auf die optischen Eigenschaften von Lithiumniobat (B07*) project PC2: Computing Resources Provided by the Paderborn Center for Parallel Computing project <jats:title>Abstract</jats:title> <jats:p>Theoretical spectroscopy based on double perturbation theory is typically challenged by systems with large orbital hyperfine splitting. Therefore, we here derive a rigorous, non-perturbative scheme starting from Dirac’s equation which allows to calculate the contribution of the orbital HFI for complex structures including heavy atoms with strong spin-orbit coupling (SOC). Using the PAW formalism, the method has been implemented in the software package Quantum ESPRESSO. We show that the ‘orbital part’ actually scales with SOC strength if orbital quenching is hindered by low local symmetry, i.e. in case of dimers or atoms at surfaces. This holds true in particular when the unpaired electron is localized in quasi-atomic <jats:italic>p</jats:italic>-like orbitals. Here, the orbital part is by far not negligible, but becomes dominant by surpassing the dipolar contribution by a factor of five.</jats:p> IOP Publishing2024 eng 1742-6588 1742-659610.1088/1742-6596/2701/1/012094 27011 @article{Franzke_Schmidt_Gerstmann_2024, title={Relativistic calculation of the orbital hyperfine splitting in complex microscopic structures}, volume={2701}, DOI={<a href="https://doi.org/10.1088/1742-6596/2701/1/012094">10.1088/1742-6596/2701/1/012094</a>}, number={1012094}, journal={Journal of Physics: Conference Series}, publisher={IOP Publishing}, author={Franzke, Katharina and Schmidt, Wolf Gero and Gerstmann, Uwe}, year={2024} } K. Franzke, W.G. Schmidt, U. Gerstmann, Journal of Physics: Conference Series 2701 (2024). Franzke, Katharina, et al. “Relativistic Calculation of the Orbital Hyperfine Splitting in Complex Microscopic Structures.” <i>Journal of Physics: Conference Series</i>, vol. 2701, no. 1, 012094, IOP Publishing, 2024, doi:<a href="https://doi.org/10.1088/1742-6596/2701/1/012094">10.1088/1742-6596/2701/1/012094</a>. Franzke, K., Schmidt, W. G., &#38; Gerstmann, U. (2024). Relativistic calculation of the orbital hyperfine splitting in complex microscopic structures. <i>Journal of Physics: Conference Series</i>, <i>2701</i>(1), Article 012094. <a href="https://doi.org/10.1088/1742-6596/2701/1/012094">https://doi.org/10.1088/1742-6596/2701/1/012094</a> Franzke, Katharina, Wolf Gero Schmidt, and Uwe Gerstmann. “Relativistic Calculation of the Orbital Hyperfine Splitting in Complex Microscopic Structures.” <i>Journal of Physics: Conference Series</i> 2701, no. 1 (2024). <a href="https://doi.org/10.1088/1742-6596/2701/1/012094">https://doi.org/10.1088/1742-6596/2701/1/012094</a>. K. Franzke, W. G. Schmidt, and U. Gerstmann, “Relativistic calculation of the orbital hyperfine splitting in complex microscopic structures,” <i>Journal of Physics: Conference Series</i>, vol. 2701, no. 1, Art. no. 012094, 2024, doi: <a href="https://doi.org/10.1088/1742-6596/2701/1/012094">10.1088/1742-6596/2701/1/012094</a>. Franzke K, Schmidt WG, Gerstmann U. Relativistic calculation of the orbital hyperfine splitting in complex microscopic structures. <i>Journal of Physics: Conference Series</i>. 2024;2701(1). doi:<a href="https://doi.org/10.1088/1742-6596/2701/1/012094">10.1088/1742-6596/2701/1/012094</a> 548562024-06-24T06:26:02Z2025-12-05T13:36:01Z