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Full-Text Articles in Physics

Molecular Interactions With Ice: Molecular Embedding, Adsorption, Detection, And Release, K D. Gibson, Grant G. Langlois, Wenxin Li, Daniel Killelea, S J. Sibener Sep 2014

Molecular Interactions With Ice: Molecular Embedding, Adsorption, Detection, And Release, K D. Gibson, Grant G. Langlois, Wenxin Li, Daniel Killelea, S J. Sibener

Chemistry: Faculty Publications and Other Works

The interaction of atomic and molecular species with water and ice is of fundamental importance for chemistry. In a previous series of publications, we demonstrated that translational energy activates the embedding of Xe and Kr atoms in the near surface region of ice surfaces. In this paper, we show that inert molecular species may be absorbed in a similar fashion.We also revisit Xe embedding, and further probe the nature of the absorption into the selvedge. CF4 molecules with high translational energies (≥3 eV) were observed to embed in amorphous solid water. Just as with Xe, the initial adsorption rate ...


On The Origin Of Mode- And Bond-Selectivity In Vibrationally Mediated Reactions On Surfaces, Daniel Killelea, Arthur L. Utz Oct 2013

On The Origin Of Mode- And Bond-Selectivity In Vibrationally Mediated Reactions On Surfaces, Daniel Killelea, Arthur L. Utz

Chemistry: Faculty Publications and Other Works

The experimental observations of vibrational mode- and bond-selective chemistry at the gas–surface interface indicate that energy redistribution within the reaction complex is not statistical on the timescale of reaction. Such behavior is a key prerequisite for efforts to use selective vibrational excitation to control chemistry at the technologically important gas–surface interface. This paper outlines a framework for understanding the origin of non-statistical reactivity on surfaces. The model focuses on the kinetic competition between intramolecular vibrational energy redistribution (IVR) within the reaction complex, which in the long-time limit leads to statistical behavior, and quenching, scattering, or desorption processes that ...