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Direct observation of ultrafast hydrogen bond strengthening in liquid water

机译：直接观察液体水中超快氢键加强

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摘要

Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network(1), including unusually efficient vibrational energy redistribution and relaxation(2). An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments(2-7). However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here, we measure the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 angstrom on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of approximately 1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on femtosecond timescales. Our experiment and simulations unveil the intermolecular character of the water vibration preceding the relaxation of the OH stretch.Liquid ultrafast electron scattering measures structural responses in liquid water with femtosecond temporal and atomic spatial resolution to reveal a transient hydrogen bond contraction then thermalization preceding relaxation of the OH stretch.
机译：水是最重要的，但最不理解的液体之一。液态水的许多异常性质源自其良好连接的氢键网络（1），包括异常有效的振动能量再分配和弛豫（2）。对水分子超快振动运动的准确描述对于了解氢键和许多溶液相化学反应的性质至关重要。在超快光谱实验（2-7）上建立了水中的大多数现有的振动松弛知识。然而，这些实验不能直接解决原子位置的运动，并且需要难以将光谱动力学翻译成氢键动态。在这里，我们使用液体超快电子散射测量液体水中液体水中浅振动振动的激发的超快结构响应。我们观察到80个飞秒的时间尺度约为0.04埃的瞬态氢键收缩，然后在大约1皮秒的时间尺度上热化。分子动力学模拟揭示了在机械上处理氢键量中的共用质子的分布，以捕获飞秒时间尺度的结构动态。我们的实验和模拟揭示了哦拉伸放松前的水振动的分子间特征。液体水中的液体水中的结构反应与飞秒的时间和原子空间分辨率，以揭示瞬态氢键收缩，然后放松前的热化。哦伸展。

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  • 来源
    《Nature》 |2021年第7873期|531-535|共5页
  • 作者

    Yang Jie; Dettori Riccardo; Nunes J. Pedro F.; List Nanna H.; Biasin Elisa; Centurion Martin; Chen Zhijiang; Cordones Amy A.; Deponte Daniel P.; Heinz Tony F.; Kozina Michael E.; Ledbetter Kathryn; Lin Ming-Fu; Lindenberg Aaron M.; Mo Mianzhen; Nilsson Anders; Shen Xiaozhe; Wolf Thomas J. A.; Donadio Davide; Gaffney Kelly J.; Martinez Todd J.; Wang Xijie;

  • 作者单位

    SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA|Tsinghua Univ Ctr Basic Mol Sci Dept Chem Beijing Peoples R China;

    Univ Calif Davis Dept Chem Davis CA USA;

    Univ Nebraska Lincoln Dept Phys Lincoln NE USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford Univ Dept Chem Stanford CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA;

    Univ Nebraska Lincoln Dept Phys Lincoln NE USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA;

    Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA;

    Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford Univ Dept Appl Phys Stanford CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA;

    Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford Univ Dept Phys Stanford CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA;

    Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford Univ Dept Mat Sci & Engn Stanford CA USA|Stanford Inst Mat & Energy Sci SLAC Natl Accelerator Lab Menlo Pk CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA;

    Stockholm Univ AlbaNova Univ Ctr Dept Phys Stockholm Sweden;

    SLAC Natl Accelerator Lab Menlo Pk CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA;

    Univ Calif Davis Dept Chem Davis CA USA;

    Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford PULSE Inst SLAC Natl Accelerator Lab Menlo Pk CA USA|Stanford Univ Dept Chem Stanford CA USA;

    SLAC Natl Accelerator Lab Menlo Pk CA USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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