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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(~3P_2) with O_2(X ~3Σ_g~?), O_2(a ~1Δ_g) and O_2(b 1Σ_g~+)
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Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(~3P_2) with O_2(X ~3Σ_g~?), O_2(a ~1Δ_g) and O_2(b 1Σ_g~+)

机译：臭氧在321至329 nm处的光解离：O（〜3P_2）与O_2（X〜3Σ_g〜？），O_2（a〜1Δ_g）和O_2（b1Σ_g〜+）的相对产率

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Product imaging of O(~3P_2) following dissociation of ozone has been used to determine the relative yields of the product channels O(~3P_2) + O_2(X ~3Σ_g~?) of ozone. All three channels are prominent at all wavelengths investigated. O_2 vibrational distributions for each channel and each wavelength are also estimated assuming Boltzmann rotational distributions. Averaged over wavelength in the measured range, the yields of the O(~3P_2) + O_2(X ~3Σ_g~?), O(~3P_2) + O_2(a ~1Δ_g), and O(~3P_2) + O_2(b ~1Σ_g~+) channels are 0.36, 0.31,and 0.34, respectively. Photofragment distributions in the spin-allowed channel O(~3P) + O_2(X ~3Σ_g~?) are compared with the results of quantum mechanical calculations on the vibronically coupled PESs of the singlet states B (optically bright) and R (repulsive). The experiments suggest that considerably more vibrational excitation and less rotational excitation occur than predicted by the quantum calculations. The rotational distributions, adjusted to fit the experimental images, suggest that the dissociation takes place from a more linear configuration than the Franck?Condon bending angle of 117°. The dissociation at most wavelengths results in a positive value of the anisotropy parameter, β, both in the experiment and in the calculations. Calculations indicate that both nonadiabatic transitions and intersystem crossings substantially reduce β below the nominal value of 2.
机译：臭氧解离后的O（〜3P_2）产物成像已用于确定臭氧的产物通道O（〜3P_2）+ O_2（X〜3Σ_g〜？）的相对产率。在研究的所有波长下，所有三个通道均突出。假设玻尔兹曼旋转分布，还估计每个通道和每个波长的O_2振动分布。在测量范围内的平均波长范围内，O（〜3P_2）+ O_2（X〜3Σ_g〜？），O（〜3P_2）+ O_2（a〜1Δ_g）和O（〜3P_2）+ O_2（b 〜1Σ_g〜+）通道分别为0.36、0.31和0.34。将自旋允许通道O（〜3P）+ O_2（X〜3Σ_g〜？）中的光碎裂分布与单峰态B（光学亮）和R（排斥）的光耦合PES的量子力学计算结果进行了比较。实验表明，与量子计算所预测的相比，发生了更多的振动激发和更少的旋转激发。调整旋转分布以适合实验图像，表明解离发生的原因是比117°的Franck？Condon弯曲角更线性的配置。无论是在实验还是在计算中，大多数波长的解离都会导致各向异性参数β为正值。计算表明，非绝热过渡和系统间交叉都将β大大降低到标称值2以下。

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