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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Collision-Free Lifetimes of SO(B~3∑~-, v' = 0, 1, and 2) and Vibrational Level Dependence of Deactivation by He
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Collision-Free Lifetimes of SO(B~3∑~-, v' = 0, 1, and 2) and Vibrational Level Dependence of Deactivation by He

机译：SO（B〜3∑〜-，v'= 0、1和2）的无碰撞寿命和He失活的振动水平依赖性

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摘要

Collision-free lifetimes and deactivation rate constants of SO(B~3∑~-, v' = 0, 1, and 2) by collisions with He have been determined. SO(X~3∑~-) was generated in the photolysis of SO_2 at 193 nm (ArF laser) and excited to a single rovibrational level of B~3∑~- with a pulsed ultraviolet laser. We recorded dispersed fluorescence spectra, and found that 0-12 (350.8 nm), 1-14 (368.5 nm), and 2-17 (401.2 nm) bands are suitable for detecting fluorescence from single vibrational level of interest. Time profiles of wavelength-resolved fluorescence were recorded at various buffer gas pressures (5-165 Torr of He). Deconvolution by the integrated phase plane method derives apparent fluorescence lifetime at a given pressure. Total pressure dependence of fluorescence decay rates leads to collision-free lifetimes and rate constants for deactivation of SO(B~3∑~-, v' = 0, 1, and 2) by collisions with He. Lifetimes of SO(B~3∑~-) have been determined to be (28 ± 2) ns (v' = 0), (30 ± 3) ns (v' = 1), and (27 ± 4) ns (v' = 2). Rate coefficients for deactivation of SO(B~3∑~-) by He have been obtained to be (6.3 ± 0.3) * 10~(-12), (3.9 ± 0.2) * 10~(-11), and (1.3 ± 0.2) * 10~(-10) in units of cm~3 molecule~(-1) s~(-1) for v' = 0, 1, and 2, respectively. To the best of our knowledge, deactivation rate constants for v' = 0 and 1 of SO(B~3∑~-) are measured for the first time in the present study. The large rate coefficient of deactivation by He and vibrational level dependence is explained by predissociation via the C~3Π state.
机译：确定了与He碰撞时SO（B〜3∑〜-，v'= 0、1，和2）的无碰撞寿命和失活速率常数。 SO（X〜3∑〜-）在193 nm的SO_2（ArF激光）光解中产生，并通过脉冲紫外激光激发到B〜3∑〜-的单个振动水平。我们记录了分散的荧光光谱，发现0-12（350.8 nm），1-14（368.5 nm）和2-17（401.2 nm）的谱带适合于从感兴趣的单个振动水平检测荧光。在各种缓冲气体压力（5-165 Torr of He）下记录了波长分辨荧光的时间曲线。通过积分相平面方法进行反卷积可以得出在给定压力下的表观荧光寿命。荧光衰减率的总压力依赖性导致无碰撞寿命和与He碰撞使SO（B〜3∑〜-，v'= 0、1和2）失活的速率常数。 SO（B〜3∑〜-）的寿命已确定为（28±2）ns（v'= 0），（30±3）ns（v'= 1）和（27±4）ns（ v'= 2）。获得的He使SO（B〜3∑〜-）失活的速率系数为（6.3±0.3）* 10〜（-12），（3.9±0.2）* 10〜（-11）和（1.3 v'分别为0、1和2时，以cm〜3分子〜（-1）s〜（-1）为单位分别为±0.2）* 10〜（-10）。据我们所知，在本研究中首次测量了v'= 0且SO（B〜3∑〜-）为1的失活速率常数。 He的高失活速率系数和振动能级依赖性是通过C〜3Π状态的预离解来解释的。

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