Abstract

Time-resolved optical double resonance (DR) spectroscopy is useful in investigating the detailed mechanisms by which molecules transfer energy from one distinct rovibrational quantum state to another, thereby elucidating aspects of chemical reactivity and energetics. The DR approach employs tunable laser excitation to prepare a molecule in a specific state and a second laser excitation step to probe subsequent collision-induced or intramolecular energy transfer. We use either infrared (IR) absorption or coherent Raman excitation for state preparation and ultraviolet (UV) laser-induced fluorescence (LIF) for detection.^[1] The emphasis in this work is on high state-specificity and sensitivity, to enable detailed modeling of the resulting kinetic and spectroscopic data and to provide insight into the intermolecular and intramolecular energy transfer processes involved.^[2] For progress in this context it is essential to develop and exploit suitable tunable laser devices and quantum electronic processes.

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