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Mechanism for Si–Si Bond Rupture in Single Molecule Junctions

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Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States
Department of Chemistry, Columbia University, New York, New York 10027, United States
§ Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
Cite this: J. Am. Chem. Soc. 2016, 138, 49, 16159–16164
Publication Date (Web):November 18, 2016
https://doi.org/10.1021/jacs.6b10700
Copyright © 2016 American Chemical Society

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    Abstract

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    The stability of chemical bonds can be studied experimentally by rupturing single molecule junctions under applied voltage. Here, we compare voltage-induced bond rupture in two Si–Si backbones: one has no alternate conductive pathway whereas the other contains an additional naphthyl pathway in parallel to the Si–Si bond. We show that in contrast to the first system, the second can conduct through the naphthyl group when the Si–Si bond is ruptured using an applied voltage. We investigate this voltage induced Si–Si bond rupture by ab initio density functional theory calculations and molecular dynamics simulations that ultimately demonstrate that the excitation of molecular vibrational modes by tunneling electrons leads to homolytic Si–Si bond rupture.

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