Thermal gating of the single molecule conductance of alkanedithiols

被引:99
作者
Haiss, W [1 ]
van Zalinge, H
Bethell, D
Ulstrup, J
Schiffrin, DJ
Nichols, RJ
机构
[1] Univ Liverpool, Dept Chem, Ctr Nanoscale Sci, Liverpool L69 7ZD, Merseyside, England
[2] Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark
基金
英国工程与自然科学研究理事会;
关键词
D O I
10.1039/b507520n
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The temperature dependence of the single molecule conductance (SMC) of alpha,omega-alkanedithiols has been investigated using a scanning tunnelling microscopy (STM) method. This is based on trapping molecules between a gold STM tip and a gold substrate and measuring directly the current across the molecule under different applied potentials. A pronounced temperature dependence of the conductance, which scales logarithmically with T-1, is observed in the temperature range between 293 and 353 K. It is proposed that the origin of this dependence is the change in distribution between molecular conformers rather than changes in either the conduction mechanism or the electronic structure of the molecule. For alkanedithiols the time averaged conformer distribution shifts to less elongated conformers at higher temperatures thus giving rise to higher conductance across the molecular bridges. This is analysed by first calculating energy differences between different conformers and then calculating their partition distribution. A simple tunnelling model is then used to calculate the temperature dependent conductance based on the conformer distribution. These findings demonstrate that charge transport through single organic molecules at ambient temperatures is a subtle and highly dynamic process that cannot be described by analysing only one molecular conformation corresponding to the lowest energy geometry of the molecule.
引用
收藏
页码:253 / 264
页数:12
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