Spatiotemporal Raman Probing of Molecular Transport in sub-2-nm Plasmonic Quasi-2D Nanochannels
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arXiv
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| Autori principali: | , , , , , , , , , , , |
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| Natura: | Preprint |
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2025
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| _version_ | 1866911185838800896 |
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| author | Liu, Haoran Jiang, Zihe Hu, Zhiwei Zhang, Banghuan He, Tao Dong, Xiaohui Sun, Chaowei Tian, Jun Jiang, Wei Hu, Huatian Chen, Wen Xu, Hongxing |
| author_facet | Liu, Haoran Jiang, Zihe Hu, Zhiwei Zhang, Banghuan He, Tao Dong, Xiaohui Sun, Chaowei Tian, Jun Jiang, Wei Hu, Huatian Chen, Wen Xu, Hongxing |
| contents | Capturing molecular dynamics in nanoconfined channels with high spatiotemporal resolution is a key challenge in nanoscience, crucial for advancing catalysis, energy conversion, and molecular sensing. Bottom-up ultrathin plasmonic nanogaps, such as nanoparticle-on-mirror (NPoM) structures, are ideal for ultrasensitive probing due to their extreme light confinement, but their perceived sealed geometry has cast doubt on the existence of accessible transport pathways. Here, counterintuitively, we demonstrate that ubiquitous ligand-capped NPoM-type nanogaps can form a natural quasi-two-dimensional nanochannel, supporting molecular transport over unprecedented length scales ($\gtrsim5$ $μ$m) with an extreme aspect ratio ($>10^3$). Using wavelength-multiplexed Raman spectroscopy, we resolve the underlying centripetal infiltration pathway with a spatial resolving power of $\sim$20 nm. This redefines the NPoM architecture as a sensitive, \textit{in-situ}, all-in-one "transport-and-probe" platform, enabling real-time, reusable monitoring of analyte with $\sim$10$^{-11}$ M. This work establishes a versatile new platform for advancing super-resolved \textit{in-situ} molecular sensing, nanoscale physicochemical studies, and on-chip nanophotofluidics. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2509_26104 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Spatiotemporal Raman Probing of Molecular Transport in sub-2-nm Plasmonic Quasi-2D Nanochannels Liu, Haoran Jiang, Zihe Hu, Zhiwei Zhang, Banghuan He, Tao Dong, Xiaohui Sun, Chaowei Tian, Jun Jiang, Wei Hu, Huatian Chen, Wen Xu, Hongxing Optics Mesoscale and Nanoscale Physics Capturing molecular dynamics in nanoconfined channels with high spatiotemporal resolution is a key challenge in nanoscience, crucial for advancing catalysis, energy conversion, and molecular sensing. Bottom-up ultrathin plasmonic nanogaps, such as nanoparticle-on-mirror (NPoM) structures, are ideal for ultrasensitive probing due to their extreme light confinement, but their perceived sealed geometry has cast doubt on the existence of accessible transport pathways. Here, counterintuitively, we demonstrate that ubiquitous ligand-capped NPoM-type nanogaps can form a natural quasi-two-dimensional nanochannel, supporting molecular transport over unprecedented length scales ($\gtrsim5$ $μ$m) with an extreme aspect ratio ($>10^3$). Using wavelength-multiplexed Raman spectroscopy, we resolve the underlying centripetal infiltration pathway with a spatial resolving power of $\sim$20 nm. This redefines the NPoM architecture as a sensitive, \textit{in-situ}, all-in-one "transport-and-probe" platform, enabling real-time, reusable monitoring of analyte with $\sim$10$^{-11}$ M. This work establishes a versatile new platform for advancing super-resolved \textit{in-situ} molecular sensing, nanoscale physicochemical studies, and on-chip nanophotofluidics. |
| title | Spatiotemporal Raman Probing of Molecular Transport in sub-2-nm Plasmonic Quasi-2D Nanochannels |
| topic | Optics Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2509.26104 |