Abstract
A significant fraction of the initial population of highly vibrationally excited oxygen molecules X 3Σg−(v⩾23) prepared by stimulated emission pumping, relaxes to much lower vibrational levels (Δv≈−9). The time scale is much shorter than the known collisional lifetimes of the intervening vibrational levels and thus a sequential single-quantum relaxation mechanism can be explicitly ruled out. State-to-state measurements after preparation of v=28 and 30 provide the final-vibrational state population distribution resulting from relaxation of these two states. For v=28(30), at least 38%(7.9%) of the initially prepared population, undergoes multiquantum vibrational relaxation. The observed multiquantum relaxation explains, at least in part, the previously reported “dark channel” for relaxation of vibrational levels higher than v=26, but does not exclude the possibility of reactive scattering (forming ozone) for the remaining fraction of highly vibrationally excited molecules. We discuss possible explanations of this startling result including V–V energy transfer, V–E energy transfer, and complex formation.
Published Version
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