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关于在强红外激光场作用下多原子分子在气相介质中的多光子吸收(MPA)和解离(MPD)巳经进行过大量的研究.但是,在固相介质中这方面的研究尚属少见.迄今为止,只有Ambartzumyan等报道的TEA-CO_2激光使冻结在隔离基体上(isolated-matrix)的SF_6分子发生选择性的光解反应,以及Karlov等用类似的方法对BCl_3分子的光解反应研究.最近我们研究了一系列固体甲酸铀酰化合物的红外光谱,发现其中UO_2~(2+)基团的反对称振动频率v_a均在912—952cm~(-1)范围,与TEA-CO_2激光支线频率相符.本文研究TEA-CO_2激光作用下,单结晶水甲酸铀酰和碱式甲酸铀酰化合物发生光解反应的共同特性,并根据实验结果,初步提出了该光解反应的可能机理,即在强红外激光场下,这些化合物可以吸收多个光子而达到具有较高能量的振动激发态,在具有还原性的甲酸根离子作用下发生光解反应.
Much research has been done on multiphoton absorption (MPA) and dissociation (MPD) of polyatomic molecules in a gaseous medium under the action of a strong infrared laser field, but studies in solid media are rare. To date, only the TEA-CO 2 laser reported by Ambartzumyan et al. Has allowed selective photolytic reaction of isolated-matrix frozen SF_6 molecules and the photolysis reaction of BCl_3 molecules by Karlov et al. In a similar manner. Recently, we investigated the IR spectra of a series of solid uranyl formate compounds and found that the antisymmetric vibrational frequencies v_a of the UO_2 ~ (2+) groups are in the range of 912-952cm -1, which is in agreement with the TEA-CO_2 laser branch frequency In this paper, the common characteristics of photolysis of single crystal uranyl formate and basic uranyl formate under the TEA-CO 2 laser are studied. According to the experimental results, the possible mechanism of photolysis reaction is proposed. Under strong infrared laser field, these compounds can absorb multiple photons to reach the excited state with higher energies, and the photolytic reaction takes place under the action of reducing formate ions.