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Condensed Matter > Soft Condensed Matter

arXiv:2212.14249 (cond-mat)
[Submitted on 29 Dec 2022 ]

Title: Momentum-Resolved Sum-Frequency Vibrational Spectroscopy of Bonded Interface Layer at Charged Water Interfaces

Title: 动量分辨的键合界面层在带电水界面的和频振动光谱学

Authors:Yao Hsiao, Ting-Han Chou, Animesh Patra, Yu-Chieh Wen
Abstract: Interface-specific hydrogen- (H-)bonding network of water next to a substrate (including air) directly controls the energy transfer and chemical reaction pathway at many charged aqueous interfaces. Yet, experimental characterization of such bonded water layer structure is still a challenge due to the presence of the ion diffuse layer. We now develop a sum-frequency (SF) spectroscopic scheme with varying photon momentums as an all-optic solution for retrieving the vibrational spectra of the bonded water layer and the diffuse layer, and hence microscopic structural and charging information about an interface. Application of the method to a charged surfactant-water interface reveals a hidden weakly-donor-H-bonded water species, suggesting an asymmetric hydration-shell structure of fully solvated surfactant headgroups. In another application to a zwitterionic phosphatidylcholine (PC) lipid monolayer-water interface, we find a highly polarized bonded water layer structure associating to the PC headgroup, while the diffuse layer contribution is experimentally proven to be negligible. Our all-optic method offers not only an in situ microscopic probe of the electrochemical and biological interfaces, but also a new opportunity for promoting these researches toward high spatial and temporal resolutions.
Abstract: 水在基底(包括空气)附近的界面特异性氢键(H-键)网络直接控制许多带电水界面的能量传递和化学反应路径。然而,由于离子扩散层的存在,对这种结合水层结构的实验表征仍然是一个挑战。我们现在开发了一种利用变化光子动量的和频(SF)光谱方案,作为一种全光学解决方案,用于检索结合水层和扩散层的振动光谱,从而获得界面的微观结构和充电信息。该方法应用于带电表面活性剂-水界面,揭示了一种隐藏的弱供体氢键水物种,表明完全溶剂化的表面活性剂头部具有不对称的水合壳结构。在另一种应用中,针对两性离子磷脂酰胆碱(PC)单层-水界面,我们发现了一个高度极化的结合水层结构,与PC头部相关,而扩散层的贡献被实验证明可以忽略不计。我们的全光学方法不仅为电化学和生物界面提供了原位显微探测手段,还为这些研究向高空间和时间分辨率的发展提供了新的机会。
Subjects: Soft Condensed Matter (cond-mat.soft) ; Chemical Physics (physics.chem-ph); Optics (physics.optics)
Cite as: arXiv:2212.14249 [cond-mat.soft]
  (or arXiv:2212.14249v1 [cond-mat.soft] for this version)
  https://doi.org/10.48550/arXiv.2212.14249
arXiv-issued DOI via DataCite

Submission history

From: Yao Hsiao [view email]
[v1] Thu, 29 Dec 2022 10:08:49 UTC (1,132 KB)
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