Molecular beam scattering from flat jets of liquid dodecane and water

Author:

Yang Walt12ORCID,Foreman Madison M.12ORCID,Saric Steven12ORCID,Wodtke Alec M.345ORCID,Wilson Kevin R.2ORCID,Neumark Daniel M.12ORCID

Affiliation:

1. Department of Chemistry University of California Berkeley California USA

2. Chemical Sciences Division Lawrence Berkeley National Laboratory Berkeley California USA

3. Department of Dynamics at Surfaces Max Planck Institute for Multidisciplinary Sciences Goettingen Germany

4. Institute for Physical Chemistry University of Goettingen Goettingen Germany

5. Institute for Advanced Studies of Energy Conversion University of Goettingen Goettingen Germany

Abstract

AbstractMolecular beam experiments in which gas molecules are scattered from liquids provide detailed, microscopic perspectives on the gas–liquid interface. Extending these methods to volatile liquids while maintaining the ability to measure product energy and angular distributions presents a significant challenge. The incorporation of flat liquid jets into molecular beam scattering experiments in our laboratory has allowed us to demonstrate their utility in uncovering dynamics in this complex chemical environment. Here, we summarize recent work on the evaporation and scattering of Ne, CD4, ND3, and D2O from a dodecane flat liquid jet and present first results on the evaporation and scattering of Ar from a cold salty water jet. In the evaporation experiments, Maxwell–Boltzmann flux distributions with a cosθ angular distribution are observed. Scattering experiments reveal both impulsive scattering (IS) and trapping followed by thermal desorption (TD). Super‐specular scattering is observed for all four species scattered from dodecane and is attributed to anisotropic momentum transfer to the liquid surface. In the IS channel, rotational excitation of the polyatomic scatterers is a significant energy sink, and these species accommodate more readily on the dodecane surface compared to Ne. Our preliminary results on cold salty water jets suggest that Ar atoms undergo some vapor‐phase collisions when evaporating from the liquid surface. Initial scattering experiments characterize the mechanisms of Ar interacting with an aqueous jet, allowing for comparison to dodecane systems.Key Points Molecular beam scattering from flat liquid jets is a powerful technique to elucidate mechanistic detail at the gas–liquid interface. Previous dodecane scattering experiments have uncovered angularly‐resolved thermal desorption fractions and energy transfer at the interface for several small molecule scatterers. Preliminary results on scattering from cold salty water reveal mechanisms of interaction between argon and an aqueous jet.

Publisher

Wiley

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