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Electron Binding in a Superatom with a Repulsive Coulomb Barrier: The Case of [Ag<sub>44</sub>(SC<sub>6</sub>H<sub>3</sub>F<sub>2</sub>)<sub>30</sub>]<sup>4–</sup> in the Gas Phase

Yuriko Tasaka, Katsunosuke Nakamura, Sami Malola, Keisuke Hirata, Kuenhee Kim, Kiichirou Koyasu, Hannu Häkkinen, Tatsuya Tsukuda

2020The Journal of Physical Chemistry Letters24 citationsDOI

Abstract

The electron binding mechanism in [Ag44(SC6H3F2)30]4– (SC6H3F2 = 3,4-difluorobenzenethiolate) tetra-anion was studied by photoelectron spectroscopy (PES), collision-induced dissociation mass spectrometry (CID-MS), and density functional theory (DFT) computations. PES showed that [Ag44(SC6H3F2)30]4– is energetically metastable with respect to electron autodetachment {[Ag44(SC6H3F2)30]3– + e–} and features a repulsive Coulomb barrier (RCB) with a height of 2.7 eV. However, CID-MS revealed that [Ag44(SC6H3F2)30]4– does not release an electron upon collisional excitation but undergoes dissociation. DFT computations performed on the known structure of [Ag44(SC6H3F2)30]4– confirmed the negative adiabatic electron affinity of [Ag44(SC6H3F2)30]3– and interpreted the experimental PE spectrum by taking into account tunneling electron photodetachment through the RCB.

Topics & Concepts

Atomic physicsElectron affinity (data page)ChemistrySuperatomDensity functional theoryElectronX-ray photoelectron spectroscopyDissociation (chemistry)Electron spectroscopyMetastabilityIonBinding energyComputational chemistryPhysicsPhysical chemistryMoleculeNuclear magnetic resonanceOrganic chemistryQuantum mechanicsNanocluster Synthesis and ApplicationsGold and Silver Nanoparticles Synthesis and ApplicationsAdvanced Nanomaterials in Catalysis
Electron Binding in a Superatom with a Repulsive Coulomb Barrier: The Case of [Ag<sub>44</sub>(SC<sub>6</sub>H<sub>3</sub>F<sub>2</sub>)<sub>30</sub>]<sup>4–</sup> in the Gas Phase | Litcius