Relaxation dynamics in the B(1/2) and C(3/2) charge transfer states of XeF in solid Ar

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Abstract
Dispersed laser induced fluorescence, and time domain measurements using the optical Kerr effect are applied to study the relaxation dynamics of Xe+F− (B 2Σ1/2 and C 2Π3/2) charge transfer states in solid Ar. Very fast vibrational relaxation is observed in the C emitting site: excitation near v=20 leads to population of v=0 of the C state in 13(±2) ps. In the B emitting site, the lower vibrational states relax sequentially. Relaxation times of 800(±30) ps for 1→0 and 250(±30) ps for 2→1, are measured directly; and 150(±30) ps for 3→2 and B(v=1, and v=0) is open to states above v=3 in the B emitting site. This fast channel has a relaxation time of 7(±1) ps and must involve multiple internal conversions among the nested electronic states in the ionic manifold. Under intense pumping, the excited population relaxes by stimulated emission. Stimulated radiative relaxation rates larger than 1.5×1011 s−1 are observed for B(v=0).