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RESEARCH PRODUCT
Electron Binding in a Superatom with a Repulsive Coulomb Barrier: The Case of [Ag44(SC6H3F2)30]4– in the Gas Phase
Kuenhee KimTatsuya TsukudaTatsuya TsukudaKiichirou KoyasuKiichirou KoyasuKeisuke HirataHannu HäkkinenSami MalolaKatsunosuke NakamuraYuriko Tasakasubject
Materials scienceSuperatomCoulomb barrierElectron010402 general chemistry01 natural sciencesMolecular physicsDissociation (chemistry)0104 chemical sciencesX-ray photoelectron spectroscopyMetastability0103 physical sciencesGeneral Materials ScienceDensity functional theoryPhysical and Theoretical Chemistry010306 general physicsCollisional excitationdescription
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.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2020-04-01 | The Journal of Physical Chemistry Letters |