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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Especially Significant New Component of N_2O Quantum Yield in the UV Photolysis of O_3 in Air
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Especially Significant New Component of N_2O Quantum Yield in the UV Photolysis of O_3 in Air

机译：空气中O_3的UV光解中N_2O量子产率的特别重要的新成分

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This paper presents an alternate three-component model for the density ([M]) and temperature (T) dependence of the N_2O quantum yields (phiN_2O),in the UV photolysis of O_3 in air,from Estupinan et al.'s (ENLCW's) high-quality experiments that were a breakthrough in the pressure and T coverage.The three components consist of a new [M]-independent component,the ENLCW-discovered [M]~1 component,and the [M]~2-dependent component found by Kajimoto and Cvetanovic.The [M]~1 component is T independent.The weak T dependence of ENLCW's phiN_2o results from the T dependence of the other two components.The agreement of the three-component model with the observed phiN_2O is much better than that of ENLCW's one-component (T-dependent linear-in-[M]) model.For example,the percentage residual for a significant two-thirds of all data is better than ±8% in the three-component model compared to only one-third for the ENLCW model.The improvements due to the three-component model are real in the sense that they are obvious despite the experimental error bars in that pressure-temperature domain where the reality is expected to reveal itself in the ENLCW experiment.Also,the new [M]-independent component is nonzero positive at a very high confidence level of 97.5%,sharply contrasting with the current perception.The [M]-independent component is especially significant despite being small compared to the dominant [M]~1 component.It implies N_2O formation from excited O_3,tentatively O_3(~3B_1),immune from ENLCW and Prasad controversy over the origin of the [M] component.In the suggested interpretation,the [M]~0 component varies linearly with [O_3] in the photolyzed O_3/air mixture.Further experiments with [O_3] fixed at various amounts,while the air density and temperature are varied,could check the interpretation.Further computational-chemistry studies to better characterize the low-lying triplet states of O_3 would also help.
机译：本文针对空气中O_3的紫外光解，从Estupinan等人的论文（ENLCW's）提出了一个替代的三组分模型，该模型针对N_2O量子产率（phiN_2O）对密度（[M]）和温度（T）的依赖性。 ）是在压力和T覆盖率方面取得突破的高质量实验。这三个组成部分包括新的[M]独立组件，ENLCW发现的[M]〜1组件和[M]〜2独立的组件[M]〜1分量与T无关。ENLCWphiN_2o的弱T依赖性来自于其他两个组分的T依赖性。三组分模型与观察到的phiN_2O的一致性非常好。优于ENLCW的单分量（T依赖于[M]线性模型）模型。例如，三分量模型中所有三分之二数据的残差百分比均优于±8％对于ENLCW模型，只有三分之二。三分量模型带来的改进是切实可行的，尽管在压力-温度域中存在实验误差线，但在ENLCW实验中实际情况会显示出来，它们还是很明显的。此外，新的[M]独立成分在97.5％的极高置信度下为非零正值，与[M]无关的成分尽管占主导地位的[M]〜1成分虽然很小，但仍然特别显着。这意味着由激发的O_3，暂时的O_3（〜3B_1）形成了N_2O，不受ENLCW和在[M]成分的起源方面存在Prasad争议。在建议的解释中，光解O_3 /空气混合物中[M]〜0成分随[O_3]线性变化。进一步的实验以[O_3]固定了不同的量，同时空气密度和温度的变化，可能会证实这一解释。进一步进行计算化学研究，以更好地表征O_3的低价三重态也将有所帮助。

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