Grants and Contributions:

Grant or Award spanning more than one fiscal year. (2017-2018 to 2022-2023)

Innovative applications of molecular beam methods will be deployed to study elementary heterogeneous (photo)chemical processes on ice surfaces which are of interest to develop molecular-level interpretations for astrophysical phenomena in the interstellar medium, for fundamental interfacial chemical dynamics and for atmospheric chemistry processes relevant to the polar boundary layer.

We propose to use a novel methodology based on a recently developed magnetically focused molecular beam source, enabling the production of water vapor highly enriched in the ortho-H 2 O nuclear spin isomers, to devise and optimize separation strategies and the transfer of ortho-H 2 O, and of the resulting spin polarisation, to the condensed phase and surfaces. Confinement effects are germane to any storage methodologies therefore, we propose to perform systematic studies of nuclear spin conversion that will shed light on intra- and inter-molecular contributions to the underlying mechanism. This may contribute to improve storage strategies thereby extending the lifetime of condensed phase water samples enriched in ortho-H 2 O. These methodological developments will set the stage for fundamental interfacial chemical dynamics, heterogeneous catalysis of nuclear spin conversion and important NMR spectroscopy applications as well as for laboratory studies of the behavior of the nuclear spin isomers of water observed in comae and protoplanetary disks.

Photochemical processes are often enhanced in molecules adsorbed onto ice surfaces due to their peculiar solvation environment. We will use thin amorphous solid water films as surrogates for the quasi-liquid layer that resides at the ice surface in the natural environment and study the surface specificity of elementary processes responsible for intense NO x photochemical fluxes that emanate from the sunlit snowpack to the boundary layer upon polar Spring. Using our molecular beam/surface spectroscopy and kinetics methodology, as well as ultrafast spectroscopic techniques, we will investigate heterogeneous NO 2 hydrolysis and photolysis in/on condensed water and provide improved mechanistic descriptions and quantitative kinetic parameters. This will advance kinetic modelling efforts of the complex coupled kinetics involved in this important natural phenomenon.

Finally, environmental cryogenic electron microscopy studies of the heterogeneous nucleation and growth of ice will reveal the role played by substrate properties and growth conditions on the structure and morphology of thin vapor-deposited ice films which contribute to the interpretation of our spectroscopic/kinetics work. They will be pursued in concert within our FQR-NT funded project, sponsored by industrial partner Rio Tinto-Alcan International Limited , on the mitigation of mineral dust emissions at the Site de Disposition des Résidus de Bauxite, Jonquière, Qc .