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Laser-induced fluorescence and fluorescence depletion spectroscopy of SCCS~-

机译:SCCS〜-的激光诱导荧光和荧光耗尽光谱

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摘要

In a discharged supersonic jet of carbon disulfide,a band system of a new species is observed by laser-induced fluorescence (LIF) spectroscopy.Rotationally resolved spectra show that the observed electronic transition is ~2II_3/2-~2II_3/2.since both sulfur and carbon atoms have even numbers of electrons,it is concluded that the spectral carrier is an ionic species.Furthermore,the spectral carrier is identified as the linear negative ion SCCS~-,where the observed electronic transition is considered to be AntiA~2II_g-AntiX~2II_u.A mass specrometric measurement also gives evidence that SCCS~- is produced in the discharged jet.The vibrational structure for the upper electronic state is determined by both LIF and fluorescence depletion spectroscopy.A dispersed fluorescence spectrum is also observed to determine the vibrational structure of the lower electronic state.Frequencies of the v_1(C-C stretching) and v_2 (C-S symmetric stretching)vibrational modes are determined for both the electronic states,which are in good agreement with the theoretically calculated values.Fluorescence decay profiles are obtained for many vibronic levels,and the excited-state dynamics is descussed based on the determined fluorescence lifetimes and results of ab initio calculations.
机译:在放电的二硫化碳超声速射流中,通过激光诱导荧光(LIF)光谱观察到了新物种的能带系统。旋转解析光谱表明,观察到的电子跃迁为〜2II_3 / 2-〜2II_3 / 2。硫和碳原子具有偶数个电子,结论是光谱载体是离子种类。此外,光谱载体被鉴定为线性负离子SCCS〜-,其中观察到的电子跃迁被认为是AntiA〜2II_g -AntiX〜2II_u。质谱测量还提供了证据,表明在排出的射流中产生了SCCS〜-。通过LIF和荧光耗尽光谱法确定了上电子态的振动结构,还观察了分散的荧光光谱以确定确定电子的v_1(CC拉伸)和v_2(CS对称拉伸)振动模式的频率nic态,与理论计算值相吻合。获得了多个振动水平的荧光衰减曲线,并基于确定的荧光寿命和从头算的结果讨论了激发态动力学。

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