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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Quantum Diffusion-Controlled Chemistry: Reactions of Atomic Hydrogen with Nitric Oxide in Solid Parahydrogen
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Quantum Diffusion-Controlled Chemistry: Reactions of Atomic Hydrogen with Nitric Oxide in Solid Parahydrogen

机译：量子扩散控制化学：固体对氢中原子氢与一氧化氮的反应

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Our group has been working to develop parahydrogen (pH(2)) matrix isolation spectroscopy as a method to study low-temperature condensed-phase reactions of atomic hydrogen with various reaction partners. Guided by the well-defined studies of cold atom chemistry in rare-gas solids, the special properties of quantum hosts such as solid pH, afford new opportunities to study the analogous chemical reactions under quantum diffusion conditions in hopes of discovering new types of chemical reaction mechanisms. In this study, we present Fourier transform infrared spectroscopic studies of the 193 nm photoinduced chemistry of nitric oxide (NO) isolated in solid pH(2) over the 1.8 to 4.3 K temperature range. Upon short-term in situ irradiation the NO readily undergoes photolysis to yield ANO, NOH, NH, NH3, H2O, and H atoms. We Map the postphotolysis reactions of mobile H atoms with NO and document first-order growth in HNO and NOH reaction products for up to 5 h after photolysis. We perform three experiments at 4.3 K and one at 1.8 K to permit the temperature dependence of the reaction kinetics to be quantified. We observe Arrhenius type behavior with a pre-exponential factor of A = 01036(2) min(-1) and E-a = 2.39(1) cm(-1). This is in sharp contrast to previous H atom reactions we have studied in Solid pH(2) that display definitively non-Arrhenius behavior. The contrasting temperature dependence measured for the H + NO reaction is likely related to the details of H atom quantum diffusion in solid pH(2) and deserves further Study.
机译：我们的小组一直在努力开发对氢（pH（2））基质分离光谱法，作为研究原子氢与各种反应伙伴的低温冷凝相反应的方法。在对稀有气体固体中冷原子化学的明确研究的指导下，量子主体的特殊性质（例如固体pH）为研究量子扩散条件下的类似化学反应提供了新的机会，以期发现新型的化学反应机制。在这项研究中，我们提出了在1.8至4.3 K温度范围内在固体pH（2）中分离出的一氧化氮（NO）的193 nm光诱导化学的傅里叶变换红外光谱研究。在短期原位照射时，NO容易发生光解，生成ANO，NOH，NH，NH3，H2O和H原子。我们绘制了移动的H原子与NO的后光解反应的图谱，并记录了HNO和NOH反应产物在光解后长达5小时的一级生长。我们在4.3 K下进行了三个实验，在1.8 K下进行了一个实验，以量化反应动力学的温度依赖性。我们观察到Arrhenius类型的行为，其前指数因子为A = 01036（2）min（-1）和E-a = 2.39（1）cm（-1）。这与之前我们在固体pH（2）中研究的H原子反应形成鲜明对比，后者显示出绝对的非阿伦尼乌斯行为。 H + NO反应的相对温度依赖性很可能与固体pH（2）中H原子量子扩散的细节有关，值得进一步研究。

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