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Elucidating the Doping Effect on the Electronic Structure of Thiolate‐Protected Silver Superatoms by Photoelectron Spectroscopy
Authors:Kuenhee Kim  Keisuke Hirata  Katsunosuke Nakamura  Hirokazu Kitazawa  Shun Hayashi  Kiichirou Koyasu  Tatsuya Tsukuda
Abstract:Gas‐phase photoelectron spectroscopy (PES) was conducted on XAg24(SPhMe2)18]? (X=Ag, Au) and YAg24(SPhMe2)18]2? (Y=Pd, Pt), which have a formal superatomic core (X@Ag12)5+ or (Y@Ag12)4+ with icosahedral symmetry. PES results show that superatomic orbitals in the (Au@Ag12)5+ core remain unshifted with respect to those in the (Ag@Ag12)5+ core, whereas the orbitals in the (Y@Ag12)4+ (Y = Pd, Pt) core shift up in energy by about 1.4 eV. The remarkable doping effect of a single Y atom (Y=Pd, Pt) on the electronic structure of the chemically modified (Ag@Ag12)5+ superatom was reproduced by theoretical calculations on simplified model systems and was ascribed to 1) the weaker binding of valence electrons in Y@(Ag+)12 compared to Ag+@(Ag+)12 due to the reduction in formal charge of the core potential, and 2) the upward shift of the apparent vacuum level due to the presence of a repulsive Coulomb barrier between YAg24(SPhMe2)18]? and electron.
Keywords:Anionen-Photoelektronenspektroskopie  Dotierungseffekte  Mehrfach geladene Anionen  Repulsive Coulomb-Barriere  Thiolat-geschü  tzte Silbercluster
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