Directed Gas-Phase Formation of the Germaniumsilylene Butterfly Molecule (Ge(μ-H 2 )Si)

Aaron M. Thomas, Beni B. Dangi, Tao Yang, G. Tarczay, Ralf I. Kaiser, Bing Jian Sun, Si Ying Chen, Agnes H.H. Chang, Thanh L. Nguyen, John F. Stanton, Alexander M. Mebel

Research output: Contribution to journalArticle

Abstract

The hitherto elusive dibridged germaniumsilylene molecule (Ge(μ-H 2 )Si) has been formed for the first time via the bimolecular gas-phase reaction of ground-state germanium atoms (Ge) with silane (SiH 4 ) under single-collision conditions. Merged with state-of-the-art electronic structure calculations, the reaction was found to proceed through initial formation of a van der Waals complex in the entrance channel, insertion of the germanium into a silicon-hydrogen bond, intersystem crossing from the triplet to the singlet surface, hydrogen migrations, and eventually elimination of molecular hydrogen via a tight exit transition state, leading to the germaniumsilylene "butterfly". This investigation provides an extraordinary peek at the largely unknown silicon-germanium chemistry on the molecular level and sheds light on the essential nonadiabatic reaction dynamics of germanium and silicon, which are quite distinct from those of the isovalent carbon system, thus offering crucial insights that reveal exotic chemistry and intriguing chemical bonding in the germanium-silicon system on the most fundamental, microscopic level.

Original languageEnglish
Pages (from-to)1264-1271
Number of pages8
JournalJournal of Physical Chemistry Letters
Volume10
Issue number6
DOIs
Publication statusPublished - Mar 21 2019

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Germanium
Silicon
germanium
Gases
vapor phases
Molecules
molecules
silicon
Hydrogen
chemistry
Silanes
hydrogen
silanes
entrances
Ground state
Electronic structure
insertion
elimination
Hydrogen bonds
Carbon

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

Directed Gas-Phase Formation of the Germaniumsilylene Butterfly Molecule (Ge(μ-H 2 )Si) . / Thomas, Aaron M.; Dangi, Beni B.; Yang, Tao; Tarczay, G.; Kaiser, Ralf I.; Sun, Bing Jian; Chen, Si Ying; Chang, Agnes H.H.; Nguyen, Thanh L.; Stanton, John F.; Mebel, Alexander M.

In: Journal of Physical Chemistry Letters, Vol. 10, No. 6, 21.03.2019, p. 1264-1271.

Research output: Contribution to journalArticle

Thomas, AM, Dangi, BB, Yang, T, Tarczay, G, Kaiser, RI, Sun, BJ, Chen, SY, Chang, AHH, Nguyen, TL, Stanton, JF & Mebel, AM 2019, ' Directed Gas-Phase Formation of the Germaniumsilylene Butterfly Molecule (Ge(μ-H 2 )Si) ', Journal of Physical Chemistry Letters, vol. 10, no. 6, pp. 1264-1271. https://doi.org/10.1021/acs.jpclett.9b00284
Thomas, Aaron M. ; Dangi, Beni B. ; Yang, Tao ; Tarczay, G. ; Kaiser, Ralf I. ; Sun, Bing Jian ; Chen, Si Ying ; Chang, Agnes H.H. ; Nguyen, Thanh L. ; Stanton, John F. ; Mebel, Alexander M. / Directed Gas-Phase Formation of the Germaniumsilylene Butterfly Molecule (Ge(μ-H 2 )Si) In: Journal of Physical Chemistry Letters. 2019 ; Vol. 10, No. 6. pp. 1264-1271.
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