High-resolution spectroscopic investigation of the systematic increase of vibrational excitation in water-containing van der Waals complexes
(2023)
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- Authors
- Supervisors
- Lauzin, Clément
- Abstract
- The in-depth comprehension of intermolecular interactions is fundamental for understanding various physical, biological, and chemical phenomena. Weakly bound complexes serve as reference systems to test this understanding. Those complexes exhibit peculiar intermolecular dynamics such as predissociation, large amplitude motions, and tunneling. Increasing vibrational excitation in such complexes can provide valuable information to characterize these dynamics. The present spectroscopic investigation aims at enriching our knowledge of van der Waals complexes containing a water molecule attached to another atmospherically relevant species, namely a nitrogen molecule or an argon atom. The spectral signatures of these were obtained in the mid and near infrared ranges using two experimental set-ups, located in Louvain-la-Neuve and Calgary (Canada), respectively. In Louvain-la-Neuve, experimental development was undertaken to improve the frequency calibration accuracy and sensitivity of the cavity-based spectrometer named FANTASIO. The combination of these two state-of-the-art unique instruments allowed to systematically increase the vibrational excitation of the OH or OD stretch modes in the N2-water and Ar-water van der Waals complexes, where water refers to H2O or D2O. Specifically, we targeted and obtained original results in the 1OD, 2OH, and 3OD stretch regions. The N2-water spectra were analyzed by considering the feasible tunneling motions inside the complex within the framework of the associated permutation inversion group. A pseudo-diatomic model was used to rationalize the spectral signatures of the Ar-water complex. Additionally, we characterized the intermolecular and predissociation dynamics in each region. The results obtained in this work pose a challenge and provide reference data for future theoretical works. The present investigation, in combination with theoretical works performed by different groups worldwide, could potentially enable the future detection of these complexes in the Earth's atmosphere.
- Affiliations
Citations
Glorieux, R. (2023). High-resolution spectroscopic investigation of the systematic increase of vibrational excitation in water-containing van der Waals complexes. https://hdl.handle.net/2078.5/233817