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• W1566152279 abstract "Tunneling chemical reactions D+H2→DH+H and D+DH→D2+H in solid HD–H2 and D2–H2 mixtures were studied in the temperature range between 4 and 8K. These reactions were initiated by UV photolysis of DI molecules doped in these solids for 30s and followed by measuring the time course of electron-spin-resonance (ESR) intensities of D and H atoms. ESR intensity of D atoms produced by the photolysis decreases but that of H atoms increases with time. Time course of the D and H intensities has the fast and slow processes. The fast process, which finishes within ∼300s after the photolysis, is assigned to the reaction of D atom with one of its nearest-neighboring H2 molecules, D(H2)n(HD)12−n→H(H2)n−1(HD)13−n or D(H2)n(D2)12−n→H(HD)(H2)n−1(D2)12−n for 12⩾n⩾1. Rate constant for the D+H2 reaction between neighboring D atom–H2 molecule pair is determined to be (7.5±0.7)×10−3s−1 in solid HD–H2 and (1.3±0.3)×10−2s−1 in D2–H2 at 4.1K, which is very close to that calculated based on the theory of chemical reaction in gas phase by Hancock et al. [J. Chem. Phys. 91, 3492 (1989)] and Takayanagi and Sato [J. Chem. Phys. 92, 2862 (1990)]. This rate constant was found to be independent of temperature up to 7K within experimental error of ±30%. The slow process is assigned to the reaction of D atom produced in a cage fully surrounded by HD or D2 molecules, D(HD)12 or D(D2)12. This D atom undergoes the D+DH reaction with one of its nearest-neighboring HD molecules in solid HD–H2 or diffuses to the neighbor of H2 molecules to allow the D+H2 reaction in solid HD–H2 and D2–H2. The former is the main channel in solid HD–H2 below 6K where D atoms diffuse very slowly, whereas the latter dominates over the former above 6K. Rate for the reactions in the slow process is independent of temperature below 6K but increases with the increase in temperature above 6K. We found that the increase is due to the increase in hopping rate of D atoms to the neighbor of H2 molecules. Rate constant for the D+DH reaction was found to be independent of temperature up to 7K as well." @default.
• W1566152279 created "2016-06-24" @default.
• W1566152279 creator A5057621103 @default.
• W1566152279 date "2006-03-02" @default.
• W1566152279 modified "2023-10-17" @default.
• W1566152279 title "Tunneling chemical reactions D+H2→DH+H and D+DH→D2+H in solid D2–H2 and HD–H2 mixtures: An electron-spin-resonance study" @default.
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• W1566152279 doi "https://doi.org/10.1063/1.2170083" @default.
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