Quantum State Resolved 3D Velocity Map Imaging of Surface-Scattered Molecules: Incident Energy Effects in HCl + Self-Assembled Monolayer Collisions
Quantum State Resolved 3D Velocity Map Imaging of Surface-Scattered Molecules: Incident Energy Effects in HCl + Self-Assembled Monolayer Collisions
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DOI：
10.1021/acs.jpcc.6b03973
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发表时间：
2016-07
影响因子：
3.7
通讯作者：
C. Hoffman;D. Nesbitt
中科院分区：
文献类型：
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作者：
C. Hoffman;D. Nesbitt
采用状态选择电离和速度图成像（VMI）方法研究了甲基封端的自组装膜（SAMs）表面的热和超热HCl（v = 0，J = 0）碰撞动力学，得到了最终三维速度分布（vx，vy，vz）随振转（v，J）量子态变化的完整2π球面度图.垂直于表面（vz）的散射HCl通量的“DC切片”提供了用于消除入射光束污染的强大工具，以及以前所未有的细节获得完全相关的3D通量加权的振转量子态+平移散射动力学。在低碰撞能量（Einc = 0.7（1）kcal/mol）下，散射动力学完全由捕获-解吸（TD）事件主导，对于这两个外部（即，平移的）和内部的（即，振转）自由度定量地跟踪SAM表面温度（TS）。在高碰撞能量（Einc = 17（1）kcal/mol）的超热散射数据提供了直接的证据...
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 2π steradian map of final 3D velocity distributions (vx, vy, vz) as a function of rovibrational (v, J) quantum state. “DC slicing” of the scattered HCl flux normal to the surface (vz) 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 (Einc ≈ 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 (TS). Hyperthermal scattering data at high collision energies (Einc ≈ 17(1) kcal/mol) provide direct eviden...