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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Inelastic Scattering of Radicals at the Gas-Ionic Liquid Interface: Probing Surface Dynamics of BMIM-Cl, BMIM-BF4, and BMIM-Tf2N by Rovibronic Scattering of NO [~2Π_(1/2)(0.5)]
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Inelastic Scattering of Radicals at the Gas-Ionic Liquid Interface: Probing Surface Dynamics of BMIM-Cl, BMIM-BF4, and BMIM-Tf2N by Rovibronic Scattering of NO [~2Π_(1/2)(0.5)]

机译：自由基在气-离子液体界面处的非弹性散射：通过NO [〜2Π_（1/2）（0.5）]的Rovibronic散射探测BMIM-Cl，BMIM-BF4和BMIM-Tf2N的表面动力学

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Quantum state resolved inelastic collision dynamics at the gas-room temperature ionic bquid (RTIL) interface have been explored by scattering of an NO projectile beam, with laser induced fluorescence (LIF) detection yielding detailed distributions in vibrational, rotational, and spin-orbit degrees of freedom. Collision energies are varied by seeding 1% NO in either first run Ne (70% Ne/30% He, 2.7(9) kcal/mol) or pure H2 (20(6) kcal/mol), with the incident NO beam skimmed and colliding at 45° with respect to the surface normal. At E - 2.7(9) kcal/mol, NO scattering in the ~2Π_(1/2) state is well characterized by a rotational Boltzmann distribution equilibrated with the surface temperature, characteristic of trapping desorption (TD) collision dynamics. At higher collision energy (￡ = 20(6) kcal/mol), however, significant rotational excitation is observed, suggesting impulsive scattering (IS) dynamics where desorption occurs before the species has achieved full thermal equilibration with the surface. NO scattering at this higher energy from a series of RTILs for a fixed organic cation (BMIM) but different sized counterions (Cr, BF4~-, Tf2N~-) reveals a systematic increase in final rotational energy with increasing size, clearly suggesting coUisional access to the anion species at the interface for short alkyl chain RTILs. Particularly noteworthy is the significant nonadiabatic excitation of the NO (~2Π_(1/2), ~2Π_(3/2)) spin-orbit states, the electronic temperature of which depends systematically both on the surface temperature as well as the anion identity of the RTIL. In analogy to NO + rare gas and NO + Ag(111) scattering studies, this imphes a strong RTIL temperature and anion dependent increase in the A' - A" difference potential energy surface experienced over the course of a typical NO + liquid interface collision trajectory.
机译：通过散射NO弹束，探索了在气体室温离子液体（RTIL）界面处的量子态解析非弹性碰撞动力学，并通过激光诱导荧光（LIF）检测产生了振动，旋转和自旋轨道度的详细分布自由。通过在初次运行的Ne（70％Ne / 30％He，2.7（9）kcal / mol）或纯H2（20（6）kcal / mol）中注入1％NO来改变碰撞能量，同时掠过入射NO束并相对于表面法线发生45°碰撞。在E-2.7（9）kcal / mol下，〜2Π_（1/2）状态的NO散射通过与表面温度平衡的旋转玻耳兹曼分布，俘获解吸（TD）碰撞动力学的特征很好地表征。然而，在较高的碰撞能量（￡ = 20（6）kcal / mol）下，观察到了明显的旋转激发，这表明在物质达到与表面的完全热平衡之前发生解吸的脉冲散射（IS）动力学。对于固定的有机阳离子（BMIM），但是尺寸不同的抗衡离子（Cr，BF4〜-，Tf2N〜-），从一系列RTIL发出的较高能量下，NO的散射显示出最终旋转能随着尺寸的增加而系统地增加，这清楚地表明了自动进入短烷基链RTIL界面处的阴离子种类。特别值得注意的是NO（〜2Π_（1/2），〜2Π_（3/2））自旋轨道状态的显着绝热激发，其电子温度系统地取决于表面温度和阴离子身份RTIL。类似于NO +稀有气体和NO + Ag（111）的散射研究，这暗示了强烈的RTIL温度和在典型的NO +液体界面碰撞过程中经历的A'-A“差势能面的阴离子依赖性增加弹道。

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