通过静电偏转制备互变异构体纯分子束
Preparation of tautomer-pure molecular beams by electrostatic deflection
AI总结：
本文提出利用强非均匀场中的静电偏转技术分离互变异构体并制备纯气相样品，以2-吡啶酮/2-羟基吡啶体系为例，结合飞秒多光子电离收集光电子能谱，为在单个互变异构体层面研究结构-功能-动力学关系奠定了基础。
摘要：
互变异构体在化学中普遍存在，通常被认为在溶液中不可分离。但（生物）化学活性具有高度的互变异构体特异性，常见的例子是氨基酸和核酸。尽管互变异构体在溶液中处于平衡状态，但在分子束的冷环境中，互变异构化的势垒通常太高而无法相互转化，因此可将互变异构体视为独立的物种。在此，我们展示了互变异构体的分离以及互变异构体纯气相样品的制备。我们以2-吡啶酮/2-羟基吡啶体系为例进行了演示，该体系是尿嘧啶和胞嘧啶中的重要结构基序。互变异构体的空间分离是通过在强非均匀场中进行静电偏转实现的。此外，我们利用飞秒多光子电离技术收集了互变异构体分辨的光电子能谱。这为在单个互变异构体层面上研究结构-功能-动力学关系铺平了道路，所使用的方法（如超快动力学实验）通常缺乏进行此类研究所需的分辨率。
英文摘要：
Tautomers are ubiquitous throughout chemistry, and typically considered inseparable in solution. Yet (bio)chemical activity is highly tautomer specific, with common examples being the amino and nucleic acids. While tautomers exist in an equilibrium in solution, in the cold environment of a molecular beam the barrier to tautomerization is typically much too high for interconversion, and tautomers can be considered separate species. Here we demonstrate the separation of tautomers and production of tautomerically-pure gas-phase samples. We show this for the 2-pyridone / 2-hydroxypyridine system, an important structural motif in both uracil and cytosine. Spatial separation of the tautomers is achieved via electrostatic deflection in strong inhomogeneous fields. We furthermore collect tautomer-resolved photoelectron spectra using femtosecond multiphoton ionization. This paves the way for studying the structure-function-dynamic relationship on the level of individual tautomers, using approaches that typically lack the resolution to do so, such as ultrafast dynamics experiments.
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