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Insight into the Heterogeneity of Longitudinal Plasmonic Field in a Nanocavity Using an Intercalated Two-Dimensional Atomic Crystal Probe with a ∼7 Å Resolution
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2022-06-19 , DOI: 10.1021/jacs.2c03081
Siyu Chen 1, 2 , Shirui Weng 1 , Yuan-Hui Xiao 3 , Pan Li 1 , Miao Qin 1, 2 , Guoliang Zhou 1, 2 , Ronglu Dong 1 , Liangbao Yang 1, 4 , De-Yin Wu 3 , Zhong-Qun Tian 3
Affiliation  

Quantitative measurement of the plasmonic field distribution is of great significance for optimizing highly efficient optical nanodevices. However, the quantitative and precise measurement of the plasmonic field distribution is still an enormous challenge. In this work, we design a unique nanoruler with a ∼7 Å spatial resolution, which is based on a two-dimensional atomic crystal where the intercalated monolayer WS2 is a surface-enhanced Raman scattering (SERS) probe and four layers of MoS2 are a reference layer in a nanoparticle-on-mirror (NPoM) structure to quantitatively and directionally probe the longitudinal plasmonic field distribution at high permittivity by the quantitative SERS intensity of WS2 located in different layers. A subnanometer two-dimensional atomic crystal was used as a spacer layer to overcome the randomness of the molecular adsorption and Raman vibration direction. Combined with comprehensive theoretical derivation, numerical calculations, and spectroscopic measurements, it is shown that the longitudinal plasmonic field in an individual nanocavity is heterogeneously distributed with an unexpectedly large intensity gradient. We analyze the SERS enhancement factor on the horizontal component, which shows a great attenuation trend in the nanocavity and further provides precise insight into the horizontal component distribution of the longitudinal plasmonic field. We also provide a direct experimental verification that the longitudinal plasmonic field decays more slowly in high dielectric constant materials. These precise experimental insights into the plasmonic field using a two-dimensional atomic crystal itself as a Raman probe may propel understanding of the nanostructure optical response and applications based on the plasmonic field distribution.

中文翻译:

使用分辨率约为 7 Å 的插层二维原子晶体探针深入了解纳米腔中纵向等离子体场的异质性

等离子体场分布的定量测量对于优化高效光学纳米器件具有重要意义。然而,等离子体场分布的定量和精确测量仍然是一个巨大的挑战。在这项工作中,我们设计了一种空间分辨率约为 7 Å 的独特纳米尺,它基于二维原子晶体,其中插层单层 WS 2是表面增强拉曼散射 (SERS) 探针和四层 MoS 2是镜上纳米粒子 (NPoM) 结构中的参考层,通过 WS 2的定量 SERS 强度定量和定向探测高介电常数下的纵向等离子体场分布位于不同的层。采用亚纳米二维原子晶体作为间隔层,克服了分子吸附和拉曼振动方向的随机性。结合综合理论推导、数值计算和光谱测量,表明单个纳米腔中的纵向等离子体场是不均匀分布的,具有出乎意料的大强度梯度。我们分析了水平分量上的 SERS 增强因子,这在纳米腔中显示出很大的衰减趋势,并进一步提供了对纵向等离子体场的水平分量分布的精确洞察。我们还提供了一个直接的实验验证,即纵向等离子体场在高介电常数材料中衰减得更慢。
更新日期:2022-06-19
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