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Non-chemisorbed gold–sulfur binding prevails in self-assembled monolayers
Nature Chemistry ( IF 19.2 ) Pub Date : 2019-03-04 , DOI: 10.1038/s41557-019-0216-y
Michael S Inkpen 1 , Zhen-Fei Liu 2 , Haixing Li 1 , Luis M Campos 3 , Jeffrey B Neaton 2 , Latha Venkataraman 1, 3
Affiliation  

Gold–thiol contacts are ubiquitous across the physical and biological sciences in connecting organic molecules to surfaces. When thiols bind to gold in self-assembled monolayers (SAMs) the fate of the hydrogen remains a subject of profound debate—with implications for our understanding of their physical properties, spectroscopic features and formation mechanism(s). Exploiting measurements of the transmission through a molecular junction, which is highly sensitive to the nature of the molecule–electrode contact, we demonstrate here that the nature of the gold–sulfur bond in SAMs can be probed via single-molecule conductance measurements. Critically, we find that SAM measurements of dithiol-terminated molecular junctions yield a significantly lower conductance than solution measurements of the same molecule. Through numerous control experiments, conductance noise analysis and transport calculations based on density functional theory, we show that the gold–sulfur bond in SAMs prepared from the solution deposition of dithiols does not have chemisorbed character, which strongly suggests that under these widely used preparation conditions the hydrogen is retained.



中文翻译:

非化学吸附的金-硫结合在自组装单分子层中占主导地位

金 - 硫醇接触在将有机分子连接到表面的物理和生物科学中无处不在。当硫醇在自组装单分子层 (SAM) 中与金结合时,氢的命运仍然是一个备受争议的主题——这对我们理解它们的物理性质、光谱特征和形成机制具有重要意义。利用对分子-电极接触性质高度敏感的分子结的传输测量,我们在此证明可以通过单分子电导测量来探测 SAM 中金硫键的性质。至关重要的是,我们发现二硫醇末端分子结的 SAM 测量产生的电导显着低于相同分子的溶液测量。通过无数次对照实验,

更新日期:2019-03-05
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