三硫氰尿酸在金(111)上的结构、自组装化学和电导率的相关性

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Surface Science Pub Date : 2024-07-26 DOI:10.1016/j.susc.2024.122556
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引用次数: 0

摘要

大多数候选的简单模型分子电子元件都由一个导电的π-共轭烃连接体和至少两个锚定基团(如硫醇或异氰酸酯)组成。研究发现,精选分子可在金表面自组装,形成一维导电结构,起到 "分子线 "的作用。此外,这些低聚物还能在金纳米粒子之间形成分子桥,从而制造出简单的分子电子器件。这就提出了一个问题:其他 π 共轭分子连接体是否也能表现出类似的行为,从而为制造电子器件提供更广泛的候选材料。三硫氰尿酸(1,3,5-三嗪-2,4,6-三硫醇,TTCA)提供了一种可能的候选材料。TTCA(C3N3(SH)3)可以三硫醇或三硫酮的形式存在,其中的氢转移到硫基上,使其在环内含有三个 C=N 基团。TTCA 在自然界中以三硫酮形式存在,但当吸附到垂直方向的 Ag(111) 上时,就会转化为三硫醇。本文利用反射吸收红外光谱(RAIRS)研究了吸附在 Au(111)上的 TTCA 的结构,发现它仍然是三硫酮异构体,但随着覆盖率的增加,其取向发生了变化。扫描隧道显微镜(STM)显示,TTCA 在金(111)上形成低聚物,形成链状和三角形结构。我们利用沉积在金纳米电极间隙中的银或金纳米粒子装置,研究了吸附剂异构体结构的差异对分子电导率的影响。结果发现,当加入 TTCA 时,两种装置都能导电,但使用银制造的装置比使用金纳米粒子制造的装置导电率高约 13 倍,这与银上形成的 π 共轭结构而金上没有形成这种结构是一致的。这意味着低聚物既能在银上形成,也能在金上形成,并有可能增加可用于制造分子电子器件的分子-金属组合的范围。
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Correlating structure, self-assembly chemistry and conductivity of trithiocyanuric acid on Au(111)

The majority of candidates for simple model molecular-electronic components consist of a conductive π-conjugated hydrocarbon linker attached to at least two anchoring groups, such as thiols or isocyanides. It has been found that select molecules self-assemble on gold surfaces, creating one-dimensional conductive structures that act as “molecular wires”. Furthermore, these oligomers can form molecular bridges between gold nanoparticles, leading to the creation of simple molecular-electronic devices. This raises the question whether other π-conjugated molecular linkers could exhibit similar behavior that might offer a broader range of candidates for fabricating electronic devices. Trithiocyanuric acid (1,3,5-triazine-2,4,6-trithiol, TTCA) provides a possible candidate. TTCA (C3N3(SH)3) can exist as a trithiol or as a trithione in which hydrogens transfer to the sulfurs so that they are present with three C=N groups within the ring. TTCA exists naturally in the trithione form but converts into a trithiol when adsorbed onto an Ag(111) where it is vertically oriented. The structure of TTCA adsorbed on Au(111) is studied here using reflection-absorption infrared spectroscopy (RAIRS) where it is found to remain as the trithione isomer, but changes orientation as the coverage increases. Scanning-tunneling microscopy (STM) reveals that TTCA oligomerizes on Au(111) to form chains and triangular structures. The influence on molecular conductivity due to the differences in the adsorbate's isomeric structure was investigated using devices comprising either silver or gold nanoparticles deposited in the gap between gold nanoelectrodes. Both devices were found to conduct when dosed with TTCA, but the devices fabricated using silver were about 13 time more conductive than those made from gold nanoparticles, consistent with the π-conjugated structure formed on silver but not on gold. This implies that oligomers form both on silver and on gold and potentially increases the range of molecule-metal combinations that might be used to fabricate molecular-electronic devices.

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来源期刊
Surface Science
Surface Science 化学-物理:凝聚态物理
CiteScore
3.30
自引率
5.30%
发文量
137
审稿时长
25 days
期刊介绍: Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.
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