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State-resolved experiments probing the dynamics in NO2#–NO2 collisions at high internal energies (17 500<E<18 000 cm−1) are reported. A sequential optical double resonance technique with sensitive laser-induced fluorescence detection has been employed for the assignment of states of NO2 in the energy range between 17 500 and 18 000 cm−1, a spectral region where the optically “bright” 2B2 state is strongly coupled to high lying (“dark”) states of the 2A1 ground state and other electronic states. Subsequently, the decay of population and polarization following rotationally inelastic and elastic collisions has been probed directly using a time- and polarization-resolved optical double resonance technique. Total depopulation rates have been determined to be about 2–3 times above the Lennard-Jones estimate. The thermally averaged state-to-state cross sections have been derived from a master equation analysis of the kinetic traces. The rate constants have been scaled by angular momentum scaling expressions base...

the journal of chemical physics

State-resolved collisional energy transfer in highly excited NO2. I. Cross sections and propensities for <i>J</i>, <i>K</i>, and mJ changing collisions

State-resolved collisional energy transfer in highly excited NO2. I. Cross sections and propensities for J, K, and mJ changing collisions