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  Contrasting Efficiency of Electron-Induced Reaction at Cu(110) in Aliphatic and Aromatic Bromides

Timm, M. J., Leung, L., Anggara, K., Lim, T., Hu, Z., Latini, S., et al. (2020). Contrasting Efficiency of Electron-Induced Reaction at Cu(110) in Aliphatic and Aromatic Bromides. Journal of the American Chemical Society, 142(20), 9453-9459. doi:10.1021/jacs.0c02851.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-8FB1-1 Version Permalink: http://hdl.handle.net/21.11116/0000-0006-8FB2-0
Genre: Journal Article

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https://dx.doi.org/10.1021/jacs.0c02851 (Publisher version)
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 Creators:
Timm, M. J.1, Author
Leung, L.1, Author
Anggara, K.1, Author
Lim, T.1, Author
Hu, Z.1, Author
Latini, S.2, 3, 4, Author              
Rubio, A.2, 3, 4, Author              
Polanyi, J. C.1, Author
Affiliations:
1Lash Miller Chemical Laboratories, Department of Chemistry and Institute of Optical Sciences, University of Toronto, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Free-Electron Laser Science, ou_persistent22              
4Department of Physics, University of Hamburg, ou_persistent22              

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 Abstract: We report a comparative study of the electron-induced reaction of pentyl bromide (PeBr) and phenyl bromide (PhBr) on Cu(110) at 4.6 K, observed by scanning tunneling microscopy (STM). The induced dissociation of the intact adsorbed molecule for both reagents occurred at an energy of 2.0 eV, producing a hydrocarbon radical and a Br atom. Electron-induced C–Br bond dissociation was found to be a single-electron process for both reagents. The impulsive two-state (I2S) model was used to describe the Br atom recoil as due to molecular excitation to a repulsive anti-bonding state, in which recoil of the dissociation products occurred due to C·Br repulsion along the prior C–Br bond direction. The measured reaction yield was 3 orders of magnitude greater for PeBr, 2.0 × 10–7 reactive events per electron, than for PhBr with a yield of 1.7 × 10–10. The low yield of dissociation products from the aromatic PhBr was attributed to the presence of two additional anionic states below the 2.0 eV energy limit, absent for the aliphatic PeBr; these additional anionic states for PhBr could provide a pathway for electron transfer to the surface in the case of the aromatic, but not the aliphatic, anion. The consequent shorter lifetime of the repulsive aromatic anion of PhBr is consistent with the observation of shorter mean recoil distance (3.2 Å) of its Br dissociation product, as compared with the markedly longer recoil (8.7 Å) of Br observed from the anion of PeBr.

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Language(s): eng - English
 Dates: 2020-03-122020-04-242020-05-20
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/jacs.0c02851
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Title: Journal of the American Chemical Society
  Other : JACS
  Abbreviation : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 142 (20) Sequence Number: - Start / End Page: 9453 - 9459 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870