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- W3201253287 abstract "Molecular beams of supersonically cooled (Tᵣₒₜ ≈ 10 K) carbon monoxide (CO) have been scattered from three low-vapor-pressure liquids (PFPE, squalane, and glycerol) over a range of surface temperatures (253–303 K), with the final rovibrational distributions probed by shot-noise-limited direct IR laser absorption methods. Specifically, the present work focuses on quantum-state-resolved scattering at low incident energies (Eᵢₙc ≤ 1.0 kcal/mol), which would normally be expected to yield pure trapping desorption (TD) dynamics with CO in complete thermal equilibrium with the liquid (Tᵣₒₜ ≈ TS). By way of contrast, the nascently scattered CO(J) exhibits both rotational (Tᵣₒₜ) and Doppler translational (TDₒₚₚ) distributions distinctly colder than TS, a phenomenon which is systematically reiterated over a wide range of liquid temperatures. To help identify the relevant collision physics responsible for this surprising subthermal behavior in CO, high-level ab initio potentials and detailed molecular dynamics simulations are explored for a series of projectiles (CO, DCl, and CO₂) with varying strengths of interaction with the liquid. At low incident energies, each of the more strongly interacting DCl and CO₂ projectiles is found to thermalize with the liquid interface (Tᵣₒₜ ≈ TS), while CO is predicted to emerge colder than the surface (Tᵣₒₜ < TS) and in remarkably quantitative agreement with experiment. Statistical analysis of the trajectories identifies that CO spends substantially less time and penetrates less deeply into the surface compared to DCl/CO₂ projectiles due to a combination of a shallow van der Waals well and a steep repulsive wall. The simulations reveal that low-energy CO does not undergo conventional trapping desorption (TD) at the gas–liquid interface but instead exhibits incomplete warming from its jet-cooled value (Tᵣₒₜ ≈ 10 K) via an unexpected subthermal impulsive scattering (STIS) pathway. The data suggest that non-equilibrium IS dynamics at low energies may play a crucial role in inelastic energy transfer and thermal accommodation at the gas–liquid interface for weakly interacting collision systems." @default.
- W3201253287 created "2021-09-27" @default.
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- W3201253287 date "2020-01-01" @default.
- W3201253287 modified "2023-09-23" @default.
- W3201253287 title "Low-Energy CO Scattering at the Gas–Liquid Interface: Experimental/Theoretical Evidence for a Novel Subthermal Impulsive Scattering (STIS) Channel" @default.
- W3201253287 hasPublicationYear "2020" @default.
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