Photoelectron Imaging Signature for Selective Formation of Icosahedral Anionic Silver Cages Encapsulating Group 5 Elements: M@Ag <sub>12</sub> <sup>–</sup> (M = V, Nb, and Ta)

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書誌事項

タイトル別名
  • Photoelectron Imaging Signature for Selective Formation of Icosahedral Anionic Silver Cages Encapsulating Group 5 Elements: M@Ag_12^– (M = V, Nb, and Ta)
公開日
2024-04-15
資源種別
journal article
権利情報
  • © 2024 The Authors
DOI
  • 10.1021/acs.jpclett.4c00775
  • 10.26434/chemrxiv-2024-jg998-v2
  • 10.26434/chemrxiv-2024-jg998
公開者
American Chemical Society

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説明

An assembly of 13 atoms can form highly symmetric architectures like those belonging to D_<3h>, O_h, D_<5h>, and I_h point groups. Here, using photoelectron imaging spectroscopy in combination with density functional theory (DFT) calculations, we present a simple yet convincing experimental signature for the selective formation of icosahedral cages of anionic silver clusters encapsulating a dopant atom of group 5 elements: M@Ag_<12>^– (M = V, Nb, and Ta). Their photoelectron images obtained at 4 eV closely resemble one another: only a single ring is observed, which is assignable to photodetachment signals from a 5-fold degenerate superatomic 1D electronic shell in the 1S^21P^61D^<10> configuration of valence electrons. The perfect degeneracy represents an unambiguous fingerprint of an icosahedral symmetry, which would otherwise be lifted in all of the other structural isomers. DFT calculations confirm that I_h forms are the most stable and that D_<5h>, O_h, and D_<3h> structures are not found even in metastable states.

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