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1.
J Am Chem Soc ; 140(46): 15804-15811, 2018 Nov 21.
Article in English | MEDLINE | ID: mdl-30371076

ABSTRACT

Heterogeneous ice nucleation is a key process in many environmental and technical fields and is of particular importance in modeling atmospheric behavior and the Earth's climate. Despite an improved understanding of how water binds at solid surfaces, no clear picture has emerged to describe how 3D ice grows from the first water layer, nor what makes a particular surface efficient at nucleating bulk ice. This study reports how water at a corrugated, hydrophilic/hydrophobic surface restructures from a complex 2D network, optimized to match the solid surface, to grow into a continuous ice film. Unlike the water networks formed on plane surfaces, the corrugated Cu(511) surface stabilizes a buckled hexagonal wetting layer containing both hydrogen acceptor and donor sites. First layer water is able to relax into an "icelike" arrangement as further water is deposited, creating an array of donor and acceptor sites with the correct spacing and corrugation to stabilize second layer ice and allow continued commensurate multilayer ice growth. Comparison to previous studies of flat surfaces indicates nanoscale corrugation strongly favors ice nucleation, implying surface corrugation will be an important aspect of the surface morphology on other natural or engineered surfaces.

2.
Nat Commun ; 8: 15357, 2017 05 08.
Article in English | MEDLINE | ID: mdl-28480890

ABSTRACT

The outcome of molecule-surface collisions can be modified by pre-aligning the molecule; however, experiments accomplishing this are rare because of the difficulty of preparing molecules in aligned quantum states. Here we present a general solution to this problem based on magnetic manipulation of the rotational magnetic moment of the incident molecule. We apply the technique to the scattering of H2 from flat and stepped copper surfaces. We demonstrate control of the molecule's initial quantum state, allowing a direct comparison of differences in the stereodynamic scattering from the two surfaces. Our results show that a stepped surface exhibits a much larger dependence of the corrugation of the interaction on the alignment of the molecule than the low-index surface. We also demonstrate an extension of the technique that transforms the set-up into an interferometer, which is sensitive to molecular quantum states both before and after the scattering event.

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