Department of Physics and Electronics, University of Puerto Rico, Humacao, Puerto Rico 00791, USA.
Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA.
J Chem Phys. 2018 Jan 14;148(2):024303. doi: 10.1063/1.5005057.
In this work, we theoretically study steady state thermoelectric transport through a single-molecule junction with a long chain-like bridge. Electron transmission through the system is computed using a tight-binding model for the bridge. We analyze dependences of thermocurrent on the bridge length in unbiased and biased systems operating within and beyond the linear response regime. It is shown that the length-dependent thermocurrent is controlled by the lineshape of electron transmission in the interval corresponding to the HOMO/LUMO transport channel. Also, it is demonstrated that electron interactions with molecular vibrations may significantly affect the length-dependent thermocurrent.
在这项工作中，我们从理论上研究了通过具有长链状桥的单分子结的稳态热电输运。通过桥的紧束缚模型计算了系统中的电子传输。我们分析了在线性响应区域内和之外工作的无偏和偏压系统中，热流对桥长的依赖关系。结果表明，长度相关的热流由对应 HOMO/LUMO 输运通道的电子传输的线形状控制。此外，还证明了电子与分子振动的相互作用可能会显著影响长度相关的热流。
