AVS 63rd International Symposium & Exhibition
    Surface Science Wednesday Sessions
       Session SS+AS-WeM

Paper SS+AS-WeM13
Capture of Hyperthermal Atoms and Molecules by Amorphous Water Ice via Ballistic Embedding

Wednesday, November 9, 2016, 12:00 pm, Room 104E

Session: Environmental Interfaces, Ambient Surfaces, and In-Operando Studies
Presenter: Grant Langlois, University of Chicago
Authors: G.G. Langlois, University of Chicago
S.J. Sibener, University of Chicago
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We present comprehensive work detailing the capture and aggregation of hyperthermal atoms and molecules (CO2, CF4, Xe, Kr) by amorphous solid water (ASW) under ultra-high vacuum conditions at 125 K, near the amorphous/crystalline transition. Using time-resolved in situ reflection-absorption infrared spectroscopy (RAIRS), the gases prepared in supersonic molecular beams with translational energies above ~3.0 eV are observed to directly embed underneath the vacuum-ice interface to become absorbed within amorphous ice films despite an inability to adsorb at 125 K. Embedding into crystalline films, when observed, is less effective. Upon embedding, resultant mobility within the ice and the strength of intermolecular interactions can yield segregation of these gases into clusters, as seen in the case of CO2. Tracing the kinetics of these embedding events under different energetic conditions allows for elucidation of the underlying dynamics, and we draw comparison between all studied gases to promote generalized conclusions in regards to empirical prediction of embedding probability. Through application of a classical model of the entrance barrier for atoms and molecules colliding with amorphous ice, we provide direct evidence for a unified connection between embedding probability and momentum of the incoming atoms and molecules; an account of all embedding data measured by our group traces a singular barrier. This work highlights the interplay between translational energy and momentum accommodation during collisions with ice; atoms and molecules can become trapped in an icy surface despite an inability to simply stick to the interface. These results are of considerable importance to studies of both the astrochemistry and evolution of interstellar bodies and dust, and detailing the capture and release of gases by permafrost relating to global climate forcing.