Bicomponent supramolecular self‐assemblies studied with tip‐enhanced Raman spectroscopy,Journal of Raman Spectroscopy

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Bicomponent supramolecular self‐assemblies studied with tip‐enhanced Raman spectroscopy
Journal of Raman Spectroscopy ( IF 2.4 ) Pub Date : 2020-09-22 , DOI: 10.1002/jrs.5995
Song Jiang ₁ , Rui Zhang ₁ , Xian‐Biao Zhang ₁ , Yang Zhang ₁ , Yao Zhang ₁ , Zhen‐Chao Dong ₁

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The formation of well‐ordered supramolecular self‐assembly based on cytosine and 4,4′‐bipyridine on Ag(111) has been investigated with subnanometer‐resolved tip‐enhanced Raman spectroscopy (TERS) using a low‐temperature ultrahigh‐vacuum scanning tunneling microscope (STM). The co‐deposition of two molecules on the Ag(111) surface held at room temperature results in well‐ordered hydrogen‐bonded monolayer islands, which transform into well‐aligned double‐stranded chains after thermal annealing. Site‐dependent TERS spectra help to identify the packing structures of molecular assemblies. The changes of molecule‐specific vibrational fingerprints across the assemblies can be clearly monitored by combining high‐resolution TERS spectra with advanced multivariate analysis. Furthermore, the peak positions and relative intensities for characteristic vibrational modes of the two molecules are found to vary due to the changes of the local hydrogen bonding and interaction environment in different molecular samples. Our findings demonstrate that TERS is sensitive to the local molecular interactions, provides new potentials to monitor the functionality of molecular architectures on demand, and opens new opportunities to probe surface chemistry at the nanoscale.

中文翻译：

尖端增强拉曼光谱研究双组分超分子自组装

利用亚纳米分辨尖端增强拉曼光谱（TERS）使用低温超高真空扫描隧道技术研究了基于胞嘧啶和4,4'-联吡啶在Ag（111）上的有序超分子自组装的形成显微镜（STM）。在室温下，两个分子在Ag（111）表面上的共沉积会导致氢键键合的单层岛排列整齐，经过热退火后，它们会转变为排列良好的双链。取决于位置的TERS光谱有助于识别分子组装的堆积结构。通过将高分辨率的TERS光谱与高级多变量分析相结合，可以清楚地监控整个装配体中特定于分子的振动指纹的变化。此外，发现由于不同分子样品中局部氢键和相互作用环境的变化，两个分子的特征振动模式的峰位置和相对强度发生变化。我们的发现表明，TERS对局部分子相互作用敏感，为按需监测分子结构的功能提供了新的潜力，并为探测纳米级表面化学提供了新的机会。

更新日期：2020-09-22

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