Hoshino Shoma, Araki Mitsunori, Ishiwata Takashi, Tsukiyama Koichi
Graduate School of Chemical Sciences and Technology, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku, Tokyo 162-8601, Japan.
Phys Chem Chem Phys. 2016 Jul 28;18(28):19464-71. doi: 10.1039/c6cp02117d. Epub 2016 Jul 5.
We report the observation of amplified spontaneous emission for the first time from the 0 ((3)P0) and 0 ((1)D2) ion-pair states of Br2 by using an optical-optical double resonance technique through the B (3)Π(0) valence state as the intermediate state. The strong infrared emission propagating along the incident laser radiation is assigned to the parallel ASE transitions from the 0 ion-pair states down to the nearby 0 ion-pair states. The subsequent UV fluorescence from the 0 states to the high vibrational levels of the ground state is also observed. By the Franck-Condon simulation of the cascade UV fluorescence, we determine the vibrational distributions in the 0 states populated by ASE, which are consistent with the intensity distribution in the dispersed infrared ASE spectrum. The lifetimes of the relevant ion-pair states are evaluated by analyzing the temporal profiles of the UV fluorescence.
我们首次通过光学 - 光学双共振技术,以B(3)Π(0)价态作为中间态,观测到了Br2的0((3)P0)和0((1)D2)离子对态的放大自发辐射。沿入射激光辐射传播的强红外发射被归因于从0离子对态到附近0离子对态的平行放大自发辐射跃迁。随后还观测到了从0态到基态高振动能级的紫外荧光。通过对级联紫外荧光的弗兰克 - 康登模拟,我们确定了由放大自发辐射填充的0态中的振动分布,这与色散红外放大自发辐射光谱中的强度分布一致。通过分析紫外荧光的时间轮廓来评估相关离子对态的寿命。