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Spatially and temporally resolved studies of electron transfer reactions in solutions and thin organic surfaces

机译:溶液和有机薄表面中电子转移反应的时空解析研究

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摘要

Understanding electron transfer (ET) on the nanoscale is important to both the frontier of fundamental science and to applications in molecular electronics. Ultrafast infrared spectroscopy and conducting probe atomic force microscopy (CP-AFM) are valuable tools in studies of temporally and spatially resolved ET reactions in solutions and surfaces. Static optical metal-metal charge transfer spectra, infrared absorption spectra at different temperatures, resonance Raman spectra, and polarized light transient spectra are employed to reveal the solvent and vibrational coupling to reverse ET in transition metal complex [(CN)5OsCNRu(NH3)5]-. Experimental evidence that the non-totally symmetric vibrational mode is populated after reverse electron transfer is presented.An electrical conduction study of nanocontacts between gold-grafted polythiophene film and conductive tip under different applied load using CP-AFM is presented. The importance of the adhesion force between a conducting probe and a conductive surface for characterization of electrical properties is demonstrated.A method to measure localized charge within a molecular circuit that shows negative differential resistance via CP-AFM is presented. The voltage region over which conduction through Au-supported 11-ferrocenylundecanethiol self-assembled monolayer (SAM) was enhanced was found to strongly correlate with the region over which the scanning probe tip experienced capacitive attraction to the surface. A mechanism involving two-step resonant hole transfer via sequential oxidation and subsequent reduction is proposed.Single-molecule electrical conduction studies are presented to evaluate how the molecular linking unit influences the tunneling efficiency in metal-Molecule-metal (m-M-m) junctions. CP-AFM was employed to compare the molecular conduction of two ð-bonded molecules, one with a single thiol linker and another with a conjugated double thiol linker at both ends of the molecules. The results demonstrating that the molecule with the conjugated double thiol linkers displays higher conduction than the non-conjugated single thiol-Au contacts are presented.The electrical conduction studies of m-M-m junctions formed between Au-supported SAMs of 1-hexanethiol, 11-ferrocenylundecanethiol, and a Pt-coated AFM tip under different compressing forces using CP-AFM are presented. The observed junction resistance had two distinct power law scaling changes with compressing force. Different scaling regions were described through the change in the area of contact, tunneling distance and structure of the film under compression.
机译:了解纳米级的电子转移(ET)对于基础科学的前沿以及分子电子学中的应用都至关重要。超快速红外光谱和传导探针原子力显微镜(CP-AFM)是研究溶液和表面中时间和空间分辨的ET反应的有价值的工具。利用静态光学金属-金属电荷转移光谱,不同温度下的红外吸收光谱,共振拉曼光谱和偏振光瞬态光谱揭示过渡金属络合物[(CN)5OsCNRu(NH3)5 ]-。实验证明了逆向电子传递后出现了非完全对称的振动模式。利用CP-AFM研究了金负载的聚噻吩薄膜与导电尖端在不同施加载荷下的纳米接触。证明了导电探针和导电表面之间的粘附力对于表征电性能的重要性。提出了一种通过CP-AFM测量分子电路中局部电荷的方法,该电荷显示出负的差分电阻。发现通过Au支撑的11-二茂铁基十一烷硫醇自组装单分子层(SAM)增强了导电的电压区域与扫描探针针尖对表面产生电容性吸引的区域密切相关。提出了一种通过顺序氧化和后续还原反应进行两步共振空穴转移的机理。提出了单分子导电研究,以评估分子连接单元如何影响金属-分子-金属(m-M-m)结中的隧穿效率。 CP-AFM用于比较两个d键合分子的分子传导,一个分子带有一个硫醇连接基,另一个分子两端带有一个共轭双硫醇连接基。结果表明,具有共轭双硫醇接头的分子显示出比非共轭单硫醇-Au接触更高的导电性.Au负载的1-己硫醇,11-二茂铁基十一烷硫醇的SAM之间形成的mMm结的电导率研究并介绍了使用CP-AFM在不同压缩力下镀有Pt的AFM尖端。观察到的结电阻具有两个明显的幂律随压缩力变化的标度变化。通过改变接触面积,隧穿距离和压缩膜的结构来描述不同的缩放区域。

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    Tivanski Alexei V.;

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  • 年度 2005
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  • 原文格式 PDF
  • 正文语种 en
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