Relaxation Behavior of Excited Small Molecules Doped in Rare Gas Crystals and Clusters

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The purpose of the present study is to investigate the relaxation behavior of small molecules doped in rare gas and/or N_2 crystals following the photon-absorption. The following results have been obtained. 1. The emission spectra from excited O_2 and/or N_2 molecules and atomic species were observed. 2. In the case of O_2 molecules diluted in a low-temperature Ar crystal, short lived c-a emissions, particlarly from the v'=5 level were observed along with the A'-X emissions. 3. In the case of O_2 molecules doped in a low temperature N_2 crystal, two emission band systems, one from the v'=1 level of A' state to X state, and the other from the v'=0 level of c state to a state were observed, independent on the excitation wavelength. 4. When a low temperature N_2 crystal was irradiated by a focused excimer laser at 248 nm, the emission from the ^2D excited state of atomic nitrogen was observed. It was concluded that N_2 molecules are excited via two-photon process and relax to A state and then transfer the excitation energy to the ground state atomic nitrogen to yield the excited nitrogen atoms. 5. In summary, various excited states of O_2 and N_2 molecules could be produced via one-and multiple-photon absorption and some excited apecies were found to be stored in the crystal for a long time.