Modeling experimental low energy ion scattering multi-angle maps with molecular FAN

CS Wong and RD Kolasinski and JA Whaley, SURFACE SCIENCE, 729, 122229 (2023).

DOI: 10.1016/j.susc.2022.122229

Multi-angle maps obtained with low energy ion scattering (LEIS) are not only a convenient way to visualize the atomic-level surface structure of single crystals, but also provide a comprehensive data set that is useful for quantitative fitting with models. However, modeling these maps is often difficult due to the complexity of the scattering process, as well as the number of simulations needed to accurately reproduce a single experimental map. For example, traditional molecular dynamics (MD) and binary collision approximation (BCA) simulations typically require on the order of one billion simulated ion trajectories to obtain sufficient statistics. This problem is exacerbated when modeling impact- collision ion scattering spectroscopy (ICISS) maps, as backscattering cross sections are much smaller than forward-scattering cross sections. A workaround to this problem was given by Neihus and Spitzl in the form of FAN (Niehus and Spitzl, 1991), a simulation that approximates the angular dependence of the backscattering signal by only simulating ion trajectories that reach and emanate from lattice atoms, using a BCA code. This greatly reduces the number of trajectories that must be calculated, though it can oversimplify some of the more complex collision sequences. In this work, we develop a fully three-dimensional FAN code that uses MD to simulate trajectories rather than the BCA. Our approach exploits the improved speed of FAN, while retaining the more accurate ion trajectory calculations of MD. We apply the MD-FAN simulation to model LEIS measurements on two surfaces. First, we benchmark our MD-FAN simulation in a comparison to a BCA simulation for 3 keV He+ incident on W(111) that has been previously reported in Wong et al. (2020). The MD-FAN map had stronger agreement with the experimental ICISS measurements than did the BCA map, despite containing nearly 100-fold fewer ion trajectories. Second, to obtain experimental data sets for a more complex surface, we perform experimental ICISS measurements using a 3 keV He+ beam on a magnetite single crystal, Fe3O4(001) to generate a multi-angle map. The simulated MD-FAN map for the Fe3O4(001) surface once again agreed well with the experimental map, allowing for quantitative comparisons. The MD-FAN simulation also provided insight into the scattering processes, revealing that some of the observed pattern arises from 3 keV He+ that have backscattered into the detector from Fe atoms more than 2 nm below the surface.

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