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• W2019732008 abstract "The surface and bulk diffusion of H218O on single-crystal H216O ice multilayers grown epitaxially on Ru(001) were measured using laser-induced thermal desorption (LITD) techniques. Low-energy electron diffraction studies confirmed that the ice multilayers on Ru(001) were crystalline to thicknesses of at least 105 bilayers (i.e., ∼385 Å). Measurements of H218O surface diffusion on the crystalline ice multilayers were performed using a scanning LITD method with mass spectrometric detection. Using a mask, one bilayer of isotopically-labeled H218O was deposited on half of a crystalline H216O ice multilayer. LITD measurements were then used to scan the coverage profile as a function of diffusion time at 140 K. No H218O LITD signals were observed on the masked half of the crystal for diffusion times as long as 60 min. These measurements were consistent with an upper limit for H218O surface diffusion of DS ≤ 5 × 10-9 cm2/s at 140 K. The lack of measurable surface diffusion may indicate that H218O is diffusing into the underlying ice multilayer. H2O bulk diffusion was investigated with a novel technique utilizing a combination of isothermal desorption/depth profiling and LITD probing. In this new method, a single bilayer of H218O was deposited on a crystalline H216O multilayer. Isothermal desorption with zero-order desorption kinetics was then employed to depth profile the ice multilayer. LITD was concurrently used to monitor the isotopes remaining in the multilayer versus time. If the ice film desorbs in a layer-by-layer fashion with zero-order desorption kinetics and no interlayer mixing, the bilayer of H218O should desorb from the ice surface in ∼7 s at 160 K. However, H218O was monitored during the desorption of the entire H216O ice multilayer. This behavior indicates that H218O is diffusing readily into the underlying ice multilayer. The bulk diffusion coefficient of H218O into crystalline ice multilayers of various thicknesses was determined to be DB = 1.5(±0.5) × 10-15 cm2/s at 160 K. Sandwich experiments with stacked multilayers confirmed that H218O was diffusing into the ice bulk with no influence from a possible “liquid-like” layer on the ice surface. An Arrhenius analysis of the temperature-dependent bulk diffusion coefficients yielded an activation energy of EB = 16.7 ± 1.6 kcal/mol and a preexponential of D0 = 9.7(±0.5) × 107 cm2/s. This diffusion activation energy is within the experimental error of some of the previous measurements at higher temperatures close to the ice melting point. When the Arrhenius diffusion parameters are extended to the stratospheric temperature range of 180−210 K, the residence time τ of a H2O molecule on the ice surface ranges from 5.4 × 10-3 s to 6.8 × 10-6 s, respectively, before diffusion into the underlying ice bulk. These diffusion measurements indicate very dynamic ice surfaces at stratospheric temperatures that may facilitate the incorporation of reactants into stratospheric clouds." @default.
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• W2019732008 date "1996-01-01" @default.
• W2019732008 modified "2023-09-23" @default.
• W2019732008 title "Surface and Bulk Diffusion of H₂¹⁸O on Single-Crystal H₂¹⁶O Ice Multilayers" @default.
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• W2019732008 doi "https://doi.org/10.1021/jp952670a" @default.
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