Spin-orbit coupling (SOC) is crucial for correct electronic structure analysis in molecules and materials, for example, in large molecular systems such as superatoms, for understanding the role of transition metals in enzymes, and when investigating the energy transfer processes in metal-organic frameworks. We extend the GFN-xTB method, popular to treat extended systems, by including SOC into the hamiltonian operator. We followed the same approach as previously reported for the density-functional tight-binding method and provide and validate the necessary parameters for all elements throughout the Periodic Table. The parameters have been obtained consistently from atomic SOC calculations using the density-functional theory. We tested them for reference structures where SOC is decisive, as in the transition metal containing heme moiety, chromophores in metal-organic frameworks, and in superatoms. Our parameterization paves the path for incorporation of SOC in the GFN-xTB based electronic structure calculations of computationally expensive molecular systems.
|Journal||Journal of Chemical Physics|
|Publication status||Published - 2023 Jan 28|
Bibliographical noteFunding Information:
We thank the Center for Information Services and High-Performance Computing (ZIH) at TU Dresden for computational resources and CRC 1415 as well as SPP 2244 for financial support.
© 2023 Author(s).
All Science Journal Classification (ASJC) codes
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry