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There is currently a strong interest in evaluating transition effects in molecular electron transfer between two molecules, molecules interacting with electronic quantum devices, or two surfaces made of two different materials. To this purpose, it is useful to calculate the following parameter: the change in the electron affinity (CEA), i.e., the energy variation of the lowest unoccupied molecular orbital (LUMO), induced by the interaction of the molecule with the surface or material. In this study, we address the case of such effects for a prototypical electron transport system, namely, the electron transfer in a benzene ring substituted with a Ru(bpy)3+ or 2,2′-bipyridine (bpy) ligand between a gold or platinum surface and the ion. To this end, we employ density functional theory (DFT) calculations on benchmark systems where the vertical electronic attachment or detachment from the metal is the only relevant factor determining the CEA. The studied Ru(bpy)3+ and bpy fragments lie at the center of benzene rings composed of ortho-phenylene (o-Ph), meta-Ph, para-Ph, and para-tert-butyl-phenylene (p-t-Bu-Ph) bridging ligands, with or without ether spacers of different lengths. Both Ru(bpy)3+ and bpy fragment were first relaxed into benzene units to provide a “starting” state with a planar Ru(bpy)3
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