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利用时间分辨 Fourier红外发射光谱仪(TR FTIR),对高振动激发的 CO(υ)向 H_2O的传能反应进行了研究.传能给体分子CO(υ)193 nm激光光解CHBr_3和O_2后的次级化学反应产生.CO(υ→υ-1)的红外发射由TR FTIR跟踪检测.实验中没有观察到H_2O的振动激发.利用光谱拟合方法,得到每一延时CO(υ=1～8)的振动布居,进而求出CO各个振动激发态的相对布居随时间的演化关系.在单量子跃迁模型的基础上,利用微分法得到室温下CO(υ=1～8)向H_2O的传能速率常数.至少有2个原因导致CO(υ)向H_2O弛豫的异常快的速率:H_2O的转动对振动能隙的补偿;CO和H_2O分子间形成一定寿命的络合物.结合SSH理论和ab initio计算,对CO向H_2O的传能机理进行了解释.
The energy transfer reaction of high vibration excited CO (υ) to H_2O was studied by using time-resolved Fourier infrared emission spectrometer (TR FTIR) The secondary chemical reaction produces. The infrared emission of CO (υ → υ-1) is tracked by TR FTIR. No vibrational excitation of H 2 O is observed in the experiment. By using spectral fitting method, 8), and then obtain the relative evolution of the relative residence time of each excited states of CO over time.On the basis of single quantum transition model, we obtain the CO (υ = 1 ~ 8) to H_2O Of the energy transfer rate constant at least two reasons for the CO (υ) to H_2O relaxation rate of abnormal fast: H_2O rotation of the vibration energy gap compensation; CO and H_2O molecules form a certain lifetime complexes. SSH theory and ab initio calculation, the energy transfer mechanism of CO to H 2 O is explained.