Adsorption of the astatine species on gold surface: a relativistic density functional theory study

Abstract

We report on first-principle based studies of the adsorption interaction of astatine species on a gold surface. These studies are aimed primarily at the support and interpretation of gas chromatographic experiments with Superheavy Elements, tennessine (Ts, $Z=117$) as the heavier homologue of At and possibly nihonium (Nh, $Z=113$) as its pseudo-homologue. The adsorption energies of elemental astatine or the corresponding monohydroxide on a stable gold (111) surface are estimated using gold clusters with up to 69 atoms in order to simulate the adsorption site. To simulate the electronic structure of $\mathrm{At}-\mathrm{A}{\mathrm{u}}_{\mathrm{n}}$ and $\mathrm{AtOH}-\mathrm{A}{\mathrm{u}}_{\mathrm{n}}$ complexes, we combine accurate shape-consistent relativistic pseudopotentials and non-collinear two-component relativistic density functional theory. The predicted adsorption energies for At and AtOH on gold are $130\pm 10$ kJ/mol and $90\pm 10$ kJ/mol, respectively.