Long-range enhancement for fluorescence and Raman spectroscopy using Ag nanoislands protected with column-structured silica overlayer

IF 3.5 3区医学 Q2 CHEMISTRY, MEDICINAL

ACS Medicinal Chemistry Letters Pub Date : 2024-10-28 DOI:10.1038/s41377-024-01655-3

Takeo Minamikawa, Reiko Sakaguchi, Yoshinori Harada, Hiroki Tanioka, Sota Inoue, Hideharu Hase, Yasuo Mori, Tetsuro Takamatsu, Yu Yamasaki, Yukihiro Morimoto, Masahiro Kawasaki, Mitsuo Kawasaki

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Abstract

We demonstrate long-range enhancement of fluorescence and Raman scattering using a dense random array of Ag nanoislands (AgNIs) coated with column-structured silica (CSS) overlayer of over 100 nm thickness, namely, remote plasmonic-like enhancement (RPE). The CSS layer provides physical and chemical protection, reducing the impact between analyte molecules and metal nanostructures. RPE plates are fabricated with high productivity using sputtering and chemical immersion in gold(I)/halide solution. The RPE plate significantly enhances Raman scattering and fluorescence, even without proximity between analyte molecules and metal nanostructures. The maximum enhancement factors are 10⁷-fold for Raman scattering and 10²-fold for fluorescence. RPE is successfully applied to enhance fluorescence biosensing of intracellular signalling dynamics in HeLa cells and Raman histological imaging of oesophagus tissues. Our findings present an interesting deviation from the conventional near-field enhancement theory, as they cannot be readily explained within its framework. However, based on the phenomenological aspects we have demonstrated, the observed enhancement is likely associated with the remote resonant coupling between the localised surface plasmon of AgNIs and the molecular transition dipole of the analyte, facilitated through the CSS structure. Although further investigation is warranted to fully understand the underlying mechanisms, the RPE plate offers practical advantages, such as high productivity and biocompatibility, making it a valuable tool for biosensing and biomolecular analysis in chemistry, biology, and medicine. We anticipate that RPE will advance as a versatile analytical tool for enhanced biosensing using Raman and fluorescence analysis in various biological contexts.

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使用柱状结构二氧化硅覆盖层保护的银纳米岛实现荧光和拉曼光谱的长程增强

我们展示了利用厚度超过 100 纳米的柱状结构二氧化硅 (CSS) 覆盖层的密集随机阵列银纳米岛 (AgNIs) 对荧光和拉曼散射的长程增强，即远程类等离子体增强 (RPE)。CSS 层提供物理和化学保护，减少分析分子与金属纳米结构之间的影响。RPE 板是利用溅射和化学浸入金（I）/卤化物溶液的方法制造的，生产率很高。即使分析物分子与金属纳米结构之间没有接近，RPE 板也能显著增强拉曼散射和荧光。拉曼散射的最大增强系数为 107 倍，荧光的最大增强系数为 102 倍。RPE 成功应用于增强 HeLa 细胞内信号动态的荧光生物传感和食道组织的拉曼组织学成像。我们的研究结果与传统的近场增强理论存在有趣的偏差，因为它们无法在传统的近场增强理论框架内轻松解释。不过，根据我们所展示的现象学方面，观察到的增强可能与 AgNIs 的局部表面等离子体和分析物的分子过渡偶极子之间的远程共振耦合有关，并通过 CSS 结构得到促进。尽管还需要进一步研究才能充分了解其基本机制，但 RPE 板具有高生产率和生物相容性等实用优势，使其成为化学、生物和医学领域生物传感和生物分子分析的重要工具。我们预计，RPE 将成为一种多功能分析工具，在各种生物环境中利用拉曼和荧光分析增强生物传感。

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来源期刊

ACS Medicinal Chemistry Letters CHEMISTRY, MEDICINAL-

CiteScore

7.30

自引率

2.40%

发文量

328

审稿时长

1 months

期刊介绍： ACS Medicinal Chemistry Letters is interested in receiving manuscripts that discuss various aspects of medicinal chemistry. The journal will publish studies that pertain to a broad range of subject matter, including compound design and optimization, biological evaluation, drug delivery, imaging agents, and pharmacology of both small and large bioactive molecules. Specific areas include but are not limited to: Identification, synthesis, and optimization of lead biologically active molecules and drugs (small molecules and biologics) Biological characterization of new molecular entities in the context of drug discovery Computational, cheminformatics, and structural studies for the identification or SAR analysis of bioactive molecules, ligands and their targets, etc. Novel and improved methodologies, including radiation biochemistry, with broad application to medicinal chemistry Discovery technologies for biologically active molecules from both synthetic and natural (plant and other) sources Pharmacokinetic/pharmacodynamic studies that address mechanisms underlying drug disposition and response Pharmacogenetic and pharmacogenomic studies used to enhance drug design and the translation of medicinal chemistry into the clinic Mechanistic drug metabolism and regulation of metabolic enzyme gene expression Chemistry patents relevant to the medicinal chemistry field.