Far-wing excitation studies on the quasimolecular transitions in the Hg-rare-gas, simple-molecule half-collisions

Mathematics – Probability

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Intramolecular Energy Transfer, Intramolecular Dynamics, Dynamics Of Van Der Waals Molecules, Fluorescence And Phosphorescence Spectra, Line And Band Widths, Shapes, And Shifts

Scientific paper

We have developed a brand-new half-collision approach to the transitory quasimolecular states in the cold and thermal atomic and molecular collisions and applied it to the Hg-rare-gas, simple-molecule system. This approach consists of (a) the far-wing excitation technique to trigger a thermal half-collision by the laser excitation of a collisional quasimolecule; and (b) the vdW technique to trigger a cold half-collision by the laser excitation of a van der Waals complex in a supersonic-jet expansion; the nascent products of those half-collisions are detected in a quantum-state-resolved fashion by another laser pulse. Measurements have been made in both the frequency and time domains. In the frequency-domain measurements, a pair of nanosecond pulses are used to measure the excitation spectra of the quasimolecule. Inspection of these spectral line shapes have realized for the first time the complete separation of the rotational- and translational-energy dependence of a quantum-state-resolved scattering probability with an extensive tuning range from an ultracold (50 mK) to a higher-thermal (1000 K) regions. Interaction potentials for the relevant colliding pairs are also extracted from those line shapes for a wide range of internuclear distances. In the time-domain measurements, a pair of femtosecond laser-pulses are used to clock the half-collision in real time, giving the important information that could never be extracted in the frequency domain. Selected results are presented to demonstrate that these half-collision techniques are combined to work as a useful tool to extract the dynamical features of the transit regions in atomic and molecular collisions.

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