A1 Journal article (refereed)
Electron Binding in a Superatom with a Repulsive Coulomb Barrier : The Case of [Ag44(SC6H3F2)30]4- in the Gas Phase (2020)

Tasaka, Y., Nakamura, K., Malola, S., Hirata, K., Kim, K., Koyasy, K., Häkkinen, H., & Tsukuda, T. (2020). Electron Binding in a Superatom with a Repulsive Coulomb Barrier : The Case of [Ag44(SC6H3F2)30]4- in the Gas Phase. Journal of Physical Chemistry Letters, 11(8), Article 3069-3074. https://doi.org/10.1021/acs.jpclett.0c00786

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Publication details

All authors or editors: Tasaka, Yuriko; Nakamura, Katsunosuke; Malola, Sami; Hirata, Keisuke; Kim, Kuenhee; Koyasy, Kiichiroy; Häkkinen, Hannu; Tsukuda, Tatsuya

Journal or series: Journal of Physical Chemistry Letters

eISSN: 1948-7185

Publication year: 2020

Volume: 11

Issue number: 8

Article number: 3069-3074

Publisher: American Chemical Society

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1021/acs.jpclett.0c00786

Publication open access: Not open

Publication channel open access: 

Additional information: The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.0c00786.

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.

Keywords: nanoparticles; clusters; silver; chemical bonds; mass spectrometry; density functional theory

Free keywords: adiabaticity; collisionally activated dissociation; excitation; photoelectron spectroscopy

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Ministry reporting: Yes

Reporting Year: 2020

JUFO rating: 3