Directed Gas-Phase Formation of the Germaniumsilylene Butterfly Molecule (Ge(μ-H2 )Si)

The Journal of Physical Chemistry Letters
Aaron M ThomasAlexander M Mebel

Abstract

The hitherto elusive dibridged germaniumsilylene molecule (Ge(μ-H2)Si) has been formed for the first time via the bimolecular gas-phase reaction of ground-state germanium atoms (Ge) with silane (SiH4) 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.

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Citations

Nov 28, 2020·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Zhenghai YangAlexander M Mebel
May 19, 2021·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Vladislav S KrasnoukhovRalf I Kaiser

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