Regensburg 2022 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 46: New Methods and Developments 3: Theory
O 46.3: Vortrag
Mittwoch, 7. September 2022, 15:30–15:45, H6
A fully periodic treatment of the chemisorption function for the analysis of adsorbate-substrate interactions — •Simiam Ghan1, Karsten Reuter1, and Harald Oberhofer2 — 1Fritz-Haber-Institut der MPG, Berlin, Germany. — 2University of Bayreuth, Bayreuth, Germany
We discuss the extension of our improved Projection-Operator Diabatization scheme POD2GS[1] to the study of electronic coupling on surfaces within periodic density-functional theory (DFT) simulations. Using POD2GS, we calculate diabatic electronic couplings Hab between adsorbate and surface bands throughout k-space. It becomes thus possible to directly calculate the chemisorption function of Newns and Anderson[2], a weighted density of states which appears often in the theoretical description of surface interactions.
Interpreting the chemisorption function within the Fermi Golden Rule yields ultrafast (spin)electron transfer lifetimes directly comparable to experiment, as we demonstrate for the case of core-excited Argon monolayers on ferromagnetic substrates Fe(110), Co(0001) and Ni(111)[3]. Our scheme reveals the importance of sampling the Brillouin zone to gain accurate and convergent electron transfer rates, and offers an array of further applications.
[1] J. Chem. Theory Comput. 2020, 16, 12, 7431-7443.
[2] Phys. Rev. 1969, 178, 1123.
[3] Phys. Rev. Lett. 2014, 112, 086801.