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Electromechanical Properties of Single Molecule Devices.

机译:单分子器件的机电性能。

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摘要

Understanding the interplay between the electrical and mechanical properties of single molecules is of fundamental importance for molecular electronics. The sensitivity of charge transport to mechanical fluctuations is a key problem in developing long lasting molecular devices. Furthermore, harnessing this response to mechanical perturbation, molecular devices which can be mechanically gated can be developed. This thesis demonstrates three examples of the unique electromechanical properties of single molecules.;First, the electromechanical properties of 1,4-benzenedithiol molecular junctions are investigate. Counterintuitively, the conductance of this molecule is found to increase by more than an order of magnitude when stretched. This conductance increase is found to be reversible when the molecular junction is compressed. The current-voltage, conductance-voltage and inelastic electron tunneling spectroscopy characteristics are used to attribute the conductance increase to a strain-induced shift in the frontier molecular orbital relative to the electrode Fermi level, leading to resonant enhancement in the conductance.;Next, the effect of stretching-induced structural changes on charge transport in DNA molecules is studied. The conductance of single DNA molecules with lengths varying from 6 to 26 base pairs is measured and found to follow a hopping transport mechanism. The conductance of DNA molecules is highly sensitive to mechanical stretching, showing an abrupt decrease in conductance at surprisingly short stretching distances, with weak dependence on DNA length. This abrupt conductance decrease is attributed to force-induced breaking of hydrogen bonds in the base pairs at the end of the DNA sequence.;Finally, the effect of small mechanical modulation of the base separation on DNA conductance is investigated. The sensitivity of conductance to mechanical modulation is studied for molecules of different sequence and length. Sequences with purine-purine stacking are found to be more responsive to modulation than purine-pyrimidine sequences. This sensitivity is attributed to the perturbation of pi-pi stacking interactions and resulting effects on the activation energy and electronic coupling for the end base pairs.
机译:理解单个分子的电气和机械性能之间的相互作用对分子电子学至关重要。电荷传输对机械波动的敏感性是开发持久分子器件的关键问题。此外,利用这种对机械扰动的响应,可以开发可以机械门控的分子装置。本论文论证了单分子独特的机电性能的三个例子。首先,研究了1,4-苯二硫醇分子连接的机电性能。与直觉相反,发现该分子的电导率在拉伸时增加了一个数量级以上。发现当分子连接被压缩时,这种电导增加是可逆的。电流-电压,电导-电压和非弹性电子隧穿光谱特性被用于将电导增加归因于应变诱导的前沿分子轨道相对于电极费米能级的位移,从而导致电导共振增强。研究了拉伸诱导的结构变化对DNA分子中电荷传输的影响。测量了长度在6至26个碱基对之间的单个DNA分子的电导,并发现其遵循跳跃传输机制。 DNA分子的电导率对机械拉伸高度敏感,在极短的拉伸距离下显示出电导率的突然降低,而对DNA长度的依赖性却很弱。这种突然的电导降低归因于力诱导的DNA序列末端碱基对中氢键的断裂。最后,研究了碱基分离的小机械调节对DNA电导的影响。对于不同序列和长度的分子,研究了电导对机械调制的敏感性。发现嘌呤-嘌呤堆积的序列比嘌呤-嘧啶序列对调节的响应性更高。这种敏感性归因于pi-pi堆积相互作用的扰动以及由此产生的对末端碱基对的活化能和电子耦合的影响。

著录项

  • 作者

    Bruot, Christopher.;

  • 作者单位

    Arizona State University.;

  • 授予单位 Arizona State University.;
  • 学科 Condensed matter physics.;Nanotechnology.
  • 学位 Ph.D.
  • 年度 2014
  • 页码 139 p.
  • 总页数 139
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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