Quantum Tunneling Enhancement of the C + H2O and C + D2O Reactions at Low Temperature

被引:39
|
作者
Hickson, Kevin M. [1 ]
Loison, Jean-Christophe [1 ]
Nunez-Reyes, Dianailys [1 ]
Mereau, Raphael [1 ]
机构
[1] Univ Bordeaux, ISM, CNRS, UMR 5255, F-33400 Talence, France
来源
关键词
ATOMIC CARBON; RATE COEFFICIENTS; MASTER EQUATION; AB-INITIO; REACTION-RATES; 64; K; WATER; TEMPERATURES; OH; KINETICS;
D O I
10.1021/acs.jpclett.6b01637
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Recent studies of neutral gas-phase reactions characterized by barriers show that certain complex forming processes involving light atoms are enhanced by quantum mechanical tunneling at low temperature. Here, we performed kinetic experiments on the activated C(P-3) + H2O reaction, observing a surprising reactivity increase below 100 K, an effect that is only partially reproduced when water is replaced by its deuterated analogue. Product measurements of H- and D-atom formation allowed us to quantify the contribution of complex stabilization to the total rate while confirming the lower tunneling efficiency of deuterium. This result, which is validated through statistical calculations of the intermediate complexes and transition states has important consequences for simulated interstellar water abundances and suggests that tunneling mechanisms could be ubiquitous in cold dense clouds.
引用
收藏
页码:3641 / 3646
页数:6
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