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首页> 外文期刊>Chemical Physics: A Journal Devoted to Experimental and Theoretical Research Involving Problems of Both a Chemical and Physical Nature >Ultrafast energy transfer and population buildup among strongly coupled and curve crossing regions of the boron oxide A ~2Π and X ~2Σ~+ states
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Ultrafast energy transfer and population buildup among strongly coupled and curve crossing regions of the boron oxide A ~2Π and X ~2Σ~+ states

机译：硼氧化物A〜2Π和X〜2Σ〜+态的强耦合和曲线交叉区域之间的超快能量转移和聚集

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Boron oxide X ~2Σ~+ chemiluminescence resulting from the reaction of boron atoms with nitrogen dioxide (NO_2) and ozone (O_3) has been studied. The reactions are characterized from 10~(-5) to 10~(-3) Torr and at P_(total)～1 Torr in order to assess rapid X→A intramolecular vibrational-to-electronic transfers including BO (X~2 Σ~+, ν"=17) + M → BO (A ~2Π_(1/2), ν'= 4) + M where M = NO_2, O_3 or a combination of these oxidants with argon, and the nature of the pressure dependent population buildup due to a possible bottleneck associated with the curve crossing of the BO X ~2 Σ~+ and A~2II states between ν' = 8 and A~2Π. At the very lowest pressures, the B + NO_2 reaction also yields emission corresponding to the BO_2 A~2Π_u-X~2 Σ~+_g band system, however, the B-O_3 reaction results only in BO~* A-X emission and produces neither BO_2 A-X emission. At elevated pressures both the B-NO_2 and B-O_3 systems yield BO_2 A-X where the excited BO_2 is formed in a two-step reaction sequence. The effects of ultrafast intramolecular energy transfer, manifest at pressures as low as 2 * 10~(-5) Torr for the B-NO_2 system, are consistent with expectations based on long-range interactions. For both B-NO_2 and B-O_3 metatheses, the BO~* A ~2Π influenced by (1) a combination of population buildup in vibrational levels ν' ≥ 9 in the vicinity of the BO~* A ~2Π X~2 Σ~+ curve crossing region and (2) near resonant energy transfer among nearly isoergic levels of the X~2 Σ~+ and A~2Π states (both ~2Π_(1/2) and ~2Π_(3/2) components). The effects observed in BO demonstrate the interaction of a highly vibrationally excited ground state molecule in th presence of a collision partner with a cross-section well in excess of that expected for gas kinetic interaction and a rate constant exceeding 10~(10) Torrs~(-1).
机译：研究了硼原子与二氧化氮（NO_2）和臭氧（O_3）反应产生的氧化硼X〜2Σ〜+化学发光。反应的特征是从10〜（-5）到10〜（-3）Torr，并在P_（total）〜1 Torr进行表征，以便评估X→A分子内振动至电子的快速转移，包括BO（X〜2Σ 〜+，ν“ = 17）+ M→BO（A〜2Π_（1/2），ν'= 4）+ M，其中M = NO_2，O_3或这些氧化剂与氩的组合，以及压力的性质由于在V'= 8和A〜2Π之间的BO X〜2Σ〜+和A〜2II状态的曲线交叉可能存在瓶颈，因此可能产生依赖的种群增长。在最低压力下，B + NO_2反应也会产生相应于BO_2 A〜2Π_u-X〜2Σ〜+ _g能带系统的发射，B-O_3反应仅导致BO〜* AX发射，而不产生BO_2 AX发射。 B-O_3系统产生BO_2 AX，其中BO_2是通过两步反应序列形成的，超快分子内能量传递的影响表现在B-NO_2系统的压力低至2 * 10〜（-5）Torr时。 ，与ex一致基于远程交互的构想。对于B-NO_2和B-O_3复分解，BO〜* A〜2Π受（1）BO〜* A〜2ΠX〜2Σ附近振动水平ν'≥9的种群增长的组合的影响在X〜2Σ〜+和A〜2Π态（〜2Π_（1/2）和〜2Π_（3/2）分量）的等等能级之间，〜+曲线交叉区域和（2）接近共振能量转移。在BO中观察到的效应表明，在碰撞伙伴的存在下，高振动激发的基态分子的相互作用的横截面远远超出了气体动力学相互作用的预期，并且速率常数超过10〜（10）Torrs〜。 （-1）。

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