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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Intermolecular Dynamics of Room-Temperature Ionic Liquids: Femtosecond Optical Kerr Effect Measurements on 1-Alkyl-3-methylimidazolium Bis((trifluoromethyl)sulfonyl)imides
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Intermolecular Dynamics of Room-Temperature Ionic Liquids: Femtosecond Optical Kerr Effect Measurements on 1-Alkyl-3-methylimidazolium Bis((trifluoromethyl)sulfonyl)imides

机译：室温离子液体的分子间动力学：飞克光学Kerr效应对1-烷基-3-甲基咪唑鎓双（（三氟甲基）磺酰基）酰亚胺的测量

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摘要

Using optically heterodyne-detected Raman-induced Kerr effect spectroscopy (OHD-RIKES) with 40 fs laser pulses, the transient birefringence in the room-temperature ionic liquids (RTILs), 1-alkyl-3-methylimidazolium bis((trifluoromethyl)sulfonyl)imides, [C_nmim]NTf_2 with n = 2, 4, 5, 6, 8, 10 (C2, C4, C5, C6, C8, C10), has been studied at room temperature and ambient pressure. Near zero delay, the OHD-RIKES response is dominated by the instantaneous electronic response. The nuclear response appears as a shoulder on the electronic response. Between 0 and 1 ps, the nuclear response is dominated by the intermolecular vibrational (nondiffusive) response. For C4, C5, C6, and C8, the 1/e time of the pseudo-exponential tail of the intermolecular response decreases with viscosity, in accord with the hydrodynamic model for vibrational dephasing. Superimposed on the OHD-RIKES response for C4, C5, and C6 is a coherent oscillation with a frequency of ～140 cm~(-1). The intermolecular vibrational spectra for these RTILs obtained from the reduced OHD-RIKES data by using a Fourier transform procedure extend from 0 to 200 cm~(-1) and are bimodal with a low-frequency component at ～22 cm~(-1) and a high-frequency component at ～84 cm~(-1). The relative contribution of the high-frequency component to the total band increases in going from C2 to C5 and remains constant for C5, C6, and C8. The behavior of the reduced spectral densities is consistent with increasing order in the liquid. It is proposed that the 140 cm~(-1) oscillation arises from collective motions of locally ordered domains in the liquid.
机译：使用具有40 fs激光脉冲的光学外差检测拉曼诱导的Kerr效应光谱（OHD-RIKES），在室温离子液体（RTIL），1-烷基-3-甲基咪唑双（双（（三氟甲基）磺酰基）中）具有瞬时双折射已经在室温和环境压力下研究了n = 2、4、5、6、8、10（C2，C4，C5，C6，C8，C10）亚胺[C_nmim] NTf_2。接近零延迟时，OHD-RIKES响应由瞬时电子响应控制。核反应似乎是电子反应的肩膀。在0 ps至1 ps之间，核反应以分子间振动（非扩散）反应为主。对于C4，C5，C6和C8，分子间响应的伪指数尾部的1 / e时间随粘度而降低，这与振动相移的流体动力学模型一致。在C4，C5和C6的OHD-RIKES响应上叠加了一个相干振荡，频率为〜140 cm〜（-1）。通过傅里叶变换程序从减少的OHD-RIKES数据获得的这些RTIL的分子间振动光谱从0扩展到200 cm〜（-1），并且是双峰的，且低频分量在〜22 cm〜（-1）处。在〜84 cm〜（-1）处有一个高频分量。从C2到C5，高频分量对整个频带的相对贡献增加，并且对于C5，C6和C8保持恒定。降低的光谱密度的行为与液体中增加的阶数一致。提出140 cm〜（-1）的振荡是由于液体中局部有序畴的集体运动引起的。

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