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    Identifying Eigen-like hydrated protons at negatively charged interfaces

    Year: 2020

    Journal: Nat. Commun., Volume 11, 1-Jan

    Authors: Tyrode, Eric; Sengupta, Sanghamitra; Sthoer, Adrien

    Organizations: Swedish Foundation for Strategic Research (SSF) through the program "Future Research Leaders-5"; Swedish Research Council (VR)Swedish Research Council; Royal Institute of Technology

    Despite the importance of the hydrogen ion in a wide range of biological, chemical, and physical processes, its molecular structure in solution remains lively debated. Progress has been primarily hampered by the extreme diffuse nature of the vibrational signatures of hydrated protons in bulk solution. Using the inherently surface-specific vibrational sum frequency spectroscopy technique, we show that at selected negatively charged interfaces, a resolved spectral feature directly linked to the H3O+ core in an Eigen-like species can be readily identified in a biologically compatible pH range. Centered at 2540cm(-1), the band is seen to shift to 1875cm(-1) when forming D3O+ upon isotopic substitution. The results offer the possibility of tracking and understanding from a molecular perspective the behavior of hydrated protons at charged interfaces. Hydrated protons are always present in aqueous solution, but their molecular structure remains under debate. Here the authors use vibrational sum frequency spectroscopy to show that at negatively charged liquid-vapor interfaces, protons adopt a specific configuration characteristic of Eigen-like species.
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