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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >~(15)N~++CD_4 and O~++~(13)CO_2 State-Selected Ion-Molecule Reactions Relevant to the Chemistry of Planetary Ionospheres
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~(15)N~++CD_4 and O~++~(13)CO_2 State-Selected Ion-Molecule Reactions Relevant to the Chemistry of Planetary Ionospheres

机译：与行星电离层化学有关的〜（15）N〜++ CD_4和O〜++〜（13）CO_2状态选择的离子分子反应

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The dissociative photoionization of N_2 and O_2 by synchrotron radiation in coincidence with threshold photoelectrons is used to produce state-selected N~+and O~+atomic ions to study their reactivity.A pure selection of their ground state,N~+(~3P)and O~+(~4S),or excited states,N~+(~1D),O~+(~2D),and O~+(~~2P),is obtained by the choice of the photon energy and by further discrimination of atomic ions produced with translational recoil energy.Both reactions studied,~(15)N~++CD4 and O~++~(13)CO_2,are of major importance for the chemistry of Titan,Mars,and Venus' ionospheres and are strongly affected by excitation of the parent atomic ion.For the reaction of N~+with methane,DCN~+and DCND~+products coming from the decomposition of a long-lived complex are surprisingly not much sensitive to the N~+excitation,whereas the branching ratio between the dissociative charge-transfer channel,leading to CD_3~+,which is the main product for the ground-state reaction,and the nondissociative charge-transfer channel,leading to CD_4~+,is completely inverted in favor of the latter wHe_n N~+is excited into the 'D state.This unanticipated result can be well understood by the spin-orbit selection rule in the N~+recombination.For the reaction of O~+with carbon dioxide,the reactive channel producing O2+,which dominates for the ground-state reaction for thermal collision energies,is completely displaced in favor of the endothermic charge-transfer channel leading to CO_2~+if either collision energy or O~+internal energy is brought to the system.The O~+(~2P)metastable state has a larger reaction cross section than the lower ~2D metastable state.Owing to the long lifetime of the N~+and O~+metastable states studied here and to their very specific reactivity,they should be individually considered in the models describing the planetary ionospheric chemistry.
机译：N_2和O_2通过同步加速器辐射与阈值光电子重合进行解离光电离，产生状态选择的N〜+和O〜+原子离子以研究其反应性。纯选择它们的基态N〜+（〜3P ）和O〜+（〜4S）或激发态N〜+（〜1D），O〜+（〜2D）和O〜+（~~ 2P）通过选择光子能量和（15）N〜++ CD4和O〜++〜（13）CO_2这两种反应对泰坦，火星和金星的化学反应都具有重要意义。对于N〜+与甲烷的反应，由长寿命配合物分解产生的DCN〜+和DCND〜+产物对N的敏感性不高，这是令人惊讶的。 〜+激发，解离电荷转移通道之间的支化比导致CD_3〜+（是基态反应的主要产物）与非解离电荷-反式导致CD_4〜+的fer通道被完全反转，而后者被NHe + n激发成'D状态。通过N〜+重组中的自旋轨道选择规则可以很好地理解这一意外结果。对于O〜+与二氧化碳的反应，生成O2 +的反应性通道（主要用于热碰撞能量的基态反应）被完全置换，有利于吸热的电荷转移通道，如果发生任何碰撞，则导致CO_2〜+能量或O〜+内部能量被带入系统.O〜+（〜2P）的可转移态比较低的〜2D亚稳态的反应截面大，由于N〜+和O〜的寿命长此处研究的+稳态及其非常特殊的反应性，应在描述行星电离层化学模型中单独考虑。

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