论文标题

底物对尖端增强的拉曼光谱的影响---频域模拟和石墨烯测量的比较

Impact of Substrate on Tip-enhanced Raman Spectroscopy --- A Comparison of Frequency Domain Simulations and Graphene Measurements

论文作者

Miranda, Hudson, Rabelo, Cassiano, Cancado, Luiz Gustavo, Vasconcelos, Thiago L., Oliveira, Bruno S., Schulz, Florian, Lange, Holger, Reich, Stephanie, Kusch, Patryk, Jorio, Ado

论文摘要

尖端增强的拉曼光谱(TERS)已达到纳米空间分辨率,以在环境条件下进行测量,并在超高真空吸尘器下进行亚纳米分辨率。已经获得了超分辨率(超出尖端顶点直径)TER,主要是在间隙模式配置中,在该配置中,导电基板将电场定位。在这里,我们提出了实验和理论上的探索,以探索负责光谱增强的现场分布。我们使用$ 40 \ pm 10 \ \ text {nm} $的金色技巧,以测量石墨烯上的ters,这是一个坐在不同底物上的空间隔离的二维样品,坐在不同的底物上:(i)玻璃,(ii)一层薄薄的金色和(iii)覆盖有$ 12 \ \ \ \ \ \ \ \ fext {分辨率是在环境条件下实现的。超分辨率是由于耦合的尖端样品 - 基底系统产生的现场配置,该系统表现出非平凡的空间表面分布。对于非差距和间隙模式配置,现场分布和对称选择规则不同。这会影响取决于拉曼模式对称性和底物结构的整体增强。

Tip-enhanced Raman spectroscopy (TERS) has reached nanometer spatial resolution for measurements performed at ambient conditions and sub-nanometer resolution at ultra high vacuum. Super-resolution (beyond the tip apex diameter) TERS has been obtained, mostly in the gap mode configuration, where a conductive substrate localizes the electric fields. Here we present experimental and theoretical TERS to explore the field distribution responsible for spectral enhancement. We use gold tips of $40\pm 10 \ \text{nm}$ apex diameter to measure TERS on graphene, a spatially delocalized two-dimensional sample, sitting on different substrates: (i) glass, (ii) a thin layer of gold and (iii) a surface covered with $12\ \text{nm}$ diameter gold spheres, for which $6\ \text{nm}$ resolution is achieved at ambient conditions. The super-resolution is due to the field configuration resulting from the coupled tip-sample-substrate system, exhibiting a non-trivial spatial surface distribution. The field distribution and the symmetry selection rules are different for non-gap vs. gap mode configurations. This influences the overall enhancement which depends on the Raman mode symmetry and substrate structure.

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