van der Poel Sebastiaan, Hurtado-Gallego Juan, Blaschke Matthias, López-Nebreda Rubén, Gallego Almudena, Mayor Marcel, Pauly Fabian, van der Zant Herre S J, Agraït Nicolás
Kavli Institute of Nanoscience, Delft University of Technology, Lorentzweg 1, Delft, 2628 CJ, The Netherlands.
Departamento de Física de la Materia Condensada, Universidad Autónoma de Madrid, Madrid, E-28049, Spain.
Nat Commun. 2024 Nov 21;15(1):10097. doi: 10.1038/s41467-024-53825-x.
Quantum interference plays an important role in charge transport through single-molecule junctions, even at room temperature. Of special interest is the measurement of the destructive quantum interference dip itself. Such measurements are especially demanding when performed in a continuous mode of operation. Here, we use mechanical modulation experiments at ambient conditions to reconstruct the destructive quantum interference dip of conductance versus displacement. Simultaneous measurements of the Seebeck coefficient show a sinusoidal response across the dip without sign change. Calculations that include electrode distance and energy alignment variations explain both observations quantitatively, emphasizing the crucial role of thermal fluctuations for measurements under ambient conditions. Our results open the way for establishing a closer link between break-junction experiments and theory in explaining single-molecule transport phenomena, especially when describing sharp features in the transmission.
量子干涉在通过单分子结的电荷传输中起着重要作用,即使在室温下也是如此。特别令人感兴趣的是对破坏性量子干涉凹陷本身的测量。当以连续操作模式进行此类测量时,要求尤其苛刻。在这里,我们在环境条件下使用机械调制实验来重建电导与位移的破坏性量子干涉凹陷。塞贝克系数的同步测量显示在凹陷处有正弦响应且符号不变。包括电极距离和能量对准变化的计算定量地解释了这两个观察结果,强调了热涨落在环境条件下测量中的关键作用。我们的结果为在解释单分子传输现象时,特别是在描述传输中的尖锐特征时,在断结实验和理论之间建立更紧密的联系开辟了道路。