†Department of Physics, University of California, Berkeley, California 94720, United States.
‡Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
Nano Lett. 2015 Jul 8;15(7):4498-503. doi: 10.1021/acs.nanolett.5b00990. Epub 2015 Jun 18.
Recent experiments have shown that transport properties of molecular-scale devices can be reversibly altered by the surrounding solvent. Here, we use a combination of first-principles calculations and experiment to explain this change in transport properties through a shift in the local electrostatic potential at the junction caused by nearby conducting and solvent molecules chemically bound to the electrodes. This effect is found to alter the conductance of 4,4'-bipyridine-gold junctions by more than 50%. Moreover, we develop a general electrostatic model that quantitatively relates the conductance and dipoles associated with the bound solvent and conducting molecules. Our work shows that solvent-induced effects can be used to control charge and energy transport at molecular-scale interfaces.
最近的实验表明，分子尺度器件的输运性质可以通过周围溶剂的作用可逆地改变。在这里，我们使用第一性原理计算和实验的结合，通过连接点处局部静电势的变化来解释输运性质的变化，这种变化是由化学结合在电极上的附近的导电和溶剂分子引起的。这种效应被发现可以使 4,4'-联吡啶-金连接的电导改变超过 50%。此外，我们还开发了一种通用的静电模型，定量地关联了与结合溶剂和导电分子相关的电导和偶极子。我们的工作表明，溶剂诱导的效应可以用于控制分子尺度界面的电荷和能量输运。
