Mechanism for Si–Si Bond Rupture in Single Molecule Junctions

详细信息    查看全文

• 作者：Haixing Li ; Nathaniel T. Kim ; Timothy A. Su ; Michael L. Steigerwald ; Colin Nuckolls ; Pierre Darancet ; James L. Leighton ; Latha Venkataraman
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：December 14, 2016
• 年：2016
• 卷：138
• 期：49
• 页码：16159-16164
• 全文大小：441K
• ISSN：1520-5126

文摘

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.