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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Quantum State Resolved 3D Velocity Map Imaging of Surface Scattered Molecules: Incident Energy Effects in HCl plus Self-Assembled Monolayer Collisions
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Quantum State Resolved 3D Velocity Map Imaging of Surface Scattered Molecules: Incident Energy Effects in HCl plus Self-Assembled Monolayer Collisions

机译：表面散射分子的量子态解析3D速度图成像：HCl和自组装单分子层碰撞中的入射能量效应

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Thermal and hyperthermal HCl (v = 0, J = 0) collision dynamics at the surface of methyl-terminated self-assembled monolayers (SAMs) are probed by state-selective ionization followed by velocity-map imaging (VMI) to yield a full 2 pi steradian map of final 3D velocity distributions (v(x), v(y), v(z)) as a function of rovibrational (v, J) quantum state. "DC slicing" of the scattered HCl flux normal to the surface (v(z)) provides a powerful tool for eliminating incident beam contamination, as well as access to fully correlated, 3D flux weighted rovibrational quantum state + translational scattering dynamics in unprecedented detail. At low collision energies (E-inc approximate to 0.7(1) kcal/mol), the scattering dynamics are completely dominated by trapping-desorption (TD) events, for which both external (i.e., translational) and internal (i.e., rovibrational) degrees of freedom quantitatively track the SAM surface temperature (T-S). Hyperthermal scattering data at high collision energies (E-inc approximate to 17(1) kcal/mol) provide direct evidence for growth of an additional nonequilibrium, impulsive scattering (IS) channel, with a strong forward scattering propensity broadly distributed around the specular angle. The competition between linear and angular momentum transfer for such a rapidly rotating hydride species (B-HCl approximate to 10 cm(-1)) is investigated in the IS channel, which reveals strong retention of translational energy with only modest rotational excitation (kappa(trans) approximate to 48(7)%, K-rot approximate to 6(2)%) and in clear contrast with studies of more slowly tumbling species (B-CO2 approximate to 0.4 cm(-1)) such as CO2 (kappa(trans) approximate to 6(2)%, kappa(rot) approximate to 20(4)%). Most importantly; the combination of (i) full 2 pi steradian angular data with (ii) full quantum state resolution permits a model free deconstruction of the experimental velocity map images into TD and IS components, which provides striking, independent confirmation of the hyperthermal yet Boltzmann-like nature of both the (i) IS quantum state and the (ii) out-of-plane momentum distributions. In summary, this novel combination of VMI with quantum state resolved scattering techniques provides powerful synergistic opportunities for correlated investigation of quantum state resolved reactive and inelastic energy transfer dynamics at gas-liquid-like interfaces with chemically "tunable" surface moieties.
机译：通过状态选择电离和速度图成像（VMI）探测甲基终止的自组装单分子层（SAM）表面的热和过热HCl（v = 0，J = 0）碰撞动力学最终3D速度分布（v（x），v（y），v（z））的pi Steradian映射作为旋转振动（v，J）量子态的函数。垂直于表面（v（z））的HCl散射通量的“ DC切片”提供了一个强大的工具，可消除入射光束的污染，并以前所未有的方式获得完全相关的3D磁通加权旋转振动量子态+平移散射动力学。在低碰撞能量（E-inc大约为0.7（1）kcal / mol）下，散射动力学完全由俘获-解吸（TD）事件控制，这两个事件的外部（即，平移）和内部（即，振动）自由度定量地跟踪SAM表面温度（TS）。高碰撞能量下的超热散射数据（E-inc大约为17（1）kcal / mol）提供了另外一个非平衡，脉冲散射（IS）通道的增长的直接证据，并且强烈的前向散射倾向广泛分布在镜面反射角附近。在IS通道中研究了这种快速旋转的氢化物物种（B-HCl大约10 cm（-1））的线性和角动量传递之间的竞争，该竞争表明仅通过适度的旋转激发（kappa（反式）约占48（7）％，钾腐烂约占6（2）％），与更慢翻滚物种（B-CO2约0.4 cm（-1））的研究形成鲜明对比，例如CO2（kappa） （反式）约为6（2）％，κ（腐烂）约为20（4）％。最重要的是; （i）完整的2 pi球面度角度数据与（ii）完整的量子态分辨率的组合允许将模型的速度图图像免费分解为TD和IS分量，从而提供了惊人的，独立的超高温但玻尔兹曼样的确认（i）IS量子态和（ii）平面外动量分布的本质。总之，这种新颖的VMI与量子态分辨散射技术的结合为在具有化学“可调”表面部分的气液样界面处的量子态分辨反应性和非弹性能量转移动力学的相关研究提供了强大的协同机会。

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