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首页> 外文期刊>The Journal of Chemical Physics >A one-photon laser induced fluorescence and a sequential two-photon optical-opticla double resonance excitation study of the vibrational structure ofthe B ~1A_1(pi pi~*) state of thiophosgene,Cl_2CS
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A one-photon laser induced fluorescence and a sequential two-photon optical-opticla double resonance excitation study of the vibrational structure ofthe B ~1A_1(pi pi~*) state of thiophosgene,Cl_2CS

机译：硫光气Cl_2CS的B〜1A_1（pi pi〜*）态振动结构的单光子激光诱导荧光和连续两光子光学光学双共振激发研究

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摘要

The vibrational structure of the AntiB ~1A_1(pi pi~*) electronic state ofet cooled thiophosgene,Cl_2CS,has been studied by laser induced fluorescence (LIF) excitation spectroscopy through the one-photon process AntiB ~1A_1<-AntiX~1A_1 adn by optical-optical double resonance (OODR),spectroscopy.Two OODR schemes were used to probe the AntiB~1A_1 state.One uses selected vibronic levels of the singlet A~1A_2(npi~*) state while the second scheme uses the companion triplet,Antia~3A_2(npi~*) as te intermediate level.The one-photon LIF and two-photon OODR shcemes use different optical selection rules and the two sets of spectra contain very different information.The analyses of the vibrational structure confirmed the existin gassignments for the Q_1(C=S stretch),Q_2(C-Cl stretch),and Q_4(out-of-plane)modes,and reversed the assignments for the Q_3(sym.Cl-C-Cl bend) and Q_6(antisym.Cl-C-Cl bend) modes.The barrier height to molecular inversion was revised upwards to 1495 cm~-1 fro an analysis of the (-)-(+) inversion splittings extracted form the vin_4=471 cm~-1 "hot" band intervals in the "warm jet" one-photon LIF spectra.The regularity of the patterns of te Dixon-Western bands and the constant connecting wave-number intervals allowed these bands to be assigned to the activity of vin_3.The loss of fluorescence and the shortening of the lifetime at higher vibrational excitation energies is attributed to the crossing ofthe AntiaB~1A_1(pipi~*) and AndiaC~1B_2(n omicron~*) electronic states at onger C=S bond distances.
机译：已通过单光子过程AntiB〜1A_1 <-AntiX〜1A_1 adn通过激光诱导荧光（LIF）激发光谱研究了冷却的硫代光气Cl_2CS AntiB〜1A_1（pi pi〜*）电子态的振动结构光学双共振（OODR），光谱学。两种OODR方案用于探测AntiB〜1A_1状态。一种方案使用选定的单线态A〜1A_2（npi〜*）的电子振动能级，而第二种方案使用伴侣三重态， Antia〜3A_2（npi〜*）为中间能级。单光子LIF和双光子OODR片使用不同的光学选择规则，两组光谱包含非常不同的信息。对振动结构的分析证实了其存在气体赋值。 Q_1（C = S拉伸），Q_2（C-Cl拉伸）和Q_4（平面外）模式，并颠倒了Q_3（符号为Cl-C-Cl弯曲）和Q_6（反符号）的分配.Cl-C-Cl弯曲）模式。通过分析，分子反演的势垒高度向上修正为1495 cm〜-1 （-）-（+）反演分裂是从“暖流”单光子LIF光谱中vin_4 = 471 cm-1的“热”能带间隔中提取的。狄克森-西能带和恒定的连接波数间隔使这些波段可以分配给vin_3的活性。在较高的振动激发能下，荧光的损失和寿命的缩短归因于AntiaB〜1A_1（pipi〜*）和AndiaC〜的交叉C = S键距离的1B_2（n omicron〜*）电子态。

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