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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Vibrational Relaxation of SO(X~3∑~-, v = 1-5) and Nascent Vibrational Distributions of SO Generated in the Photolysis of SO2 at 193.3 nm
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Vibrational Relaxation of SO(X~3∑~-, v = 1-5) and Nascent Vibrational Distributions of SO Generated in the Photolysis of SO2 at 193.3 nm

机译：SO（X〜3∑〜-，v = 1-5）的振动弛豫和SO2在193.3 nm的光解中生成的SO的新生振动分布

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摘要

Rate coefficients for deactivation of SO(X~3∑~-, v = 1-5) by collisions with SO_2 and nascent vibrational populations in v = 0-2 in the photolysis of SO_2 at 193.3 nm have been determined. A single vibrational level of SO(X~3∑~-) was detected with laser-induced fluorescence (LIF) excited via the B~3∑~--X~3∑~- system. Time-dependent profiles of LIF signals were recorded as a function of the pressures of SO_2. Observed profiles were analyzed by the integrated-profiles method and reproduced well by convolution calculations. Overall rate coefficients for vibrational relaxation of SO(v) by SO_2 have been determined to be (4.7 ± 0.5) * 10~(-12) (v = 1), (6.7 ± 0.4) * 10~(-12) (v = 2), (7.2 ± 0.7) * 10~(-12) (v = 3), (6.1 ± 1.0) * 10~(-12) (v = 4), and (8.6 ± 0.7) * 10~(-12) (v = 5) in units of cm3 molecule-1 s-1 (the quoted errors are 2). We have also found that 63% of the vibrational deactivations of v = 2 by SO_2 are governed by double-quantum relaxation: (4.2 ± 0.9) * 10~(-12) cm~3 molecule~(-1) s~(-1) for v = 2 v = 0 and (2.5 ± 0.9) * 10~(-12) cm~3 molecule~(-1) s~(-1) for v = 2 → v = 1. Ab initio calculations enable us to find two stable complexes: OS-OSO and SO-SO_2, indicating that attractive interactions play a significant role in the relaxation. The nascent vibrational distributions of SO have been measured to be 0.52 ± 0.1/0.75 ± 0.1/1.0 for v = 0/1/2. The differences in vibrational distributions reported by bulk and beam experiments are attributed to the difference in the temperature of parent SO_2.
机译：确定了SO_2在193.3 nm处的光解过程中与SO_2的碰撞和新生的振动种群在v = 0-2中的失活速率系数（X〜3∑〜-，v = 1-5）。通过B〜3∑〜--X〜3∑〜-系统激发的激光诱导荧光（LIF）检测到SO（X〜3∑〜-）的单个振动水平。记录了LIF信号随时间变化的曲线，该曲线是SO_2压力的函数。观察到的剖面通过综合剖面法进行了分析，并通过卷积计算得到了很好的再现。确定SO_2对SO（v）的振动弛豫的总速率系数为（4.7±0.5）* 10〜（-12）（v = 1），（6.7±0.4）* 10〜（-12）（v = 2），（7.2±0.7）* 10〜（-12）（v = 3），（6.1±1.0）* 10〜（-12）（v = 4）和（8.6±0.7）* 10〜（ -12）（v = 5），单位为cm3分子-1 s-1（引用的误差为2）。我们还发现，SO_2对v = 2的振动失活的63％由双量子弛豫控制：（4.2±0.9）* 10〜（-12）cm〜3分子〜（-1）s〜（- 1）对于v = 2 v = 0和（2.5±0.9）* 10〜（-12）cm〜3分子〜（-1）s〜（-1）对于v = 2→v = 1。我们找到了两个稳定的复合物：OS-OSO和SO-SO_2，表明有吸引力的相互作用在松弛中起着重要作用。对于v = 0/1/2，SO的新生振动分布已测量为0.52±0.1 / 0.75±0.1 / 1.0。本体和梁实验报告的振动分布差异归因于母体SO_2的温度差异。

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