Ellipsometric Study of the Ice Surface Structure Just Below the Melting Point

Furukawa, Y.; Yamamoto, M.; Kuroda, Toshio

doi:10.1051/jphyscol:1987168

Cited by 9 publications

(6 citation statements)

References 5 publications

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“…There is strong experimental evidence of a liquidlike layer on ice/vapor and ice/solid interfaces. Such a layer was found in NMR experiments by Kvlividze et al and Mizuno and Hanafuza, using optical ellipsometry by Furukawa et al., , in glancing-angle X-ray scattering by Kouchi et al and Dosch et al and using scanning force microscopy by Nickolayev and Petrenko and by Petrenko . In the presence of such a liquidlike layer a part of the screening charge is localized inside the liquid (or quasi-liquid) layer.…”

Section: Other Mechanisms and Approximationsmentioning

confidence: 87%

Surface States of Charge Carriers and Electrical Properties of the Surface Layer of Ice

Petrenko

Рыжкин

1997

J. Phys. Chem. B

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We propose a theoretical model that successfully describes numerically such major features of the electrical conductivity of the surface of ice as its magnitude and frequency dependence. Comparison of the model with experimental results on σs confirms that the magnitudes of the ice surface charge density and ice surface potential are close to those observed in independent measurements. The model predicts the thickness of an electric double layer which is comparable with the experimentally observed thickness of the liquidlike layer on ice (∼5 nm at −10 °C). This coincidence raises a question about the role of electrostatic pressure and possible superionic transition in the specific structure and properties of the surface of ice.

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Section: Other Mechanisms and Approximationsmentioning

confidence: 87%

Surface States of Charge Carriers and Electrical Properties of the Surface Layer of Ice

Petrenko

Рыжкин

1997

J. Phys. Chem. B

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“…One manifestation of this perturbation is the "quasi-liquid" layer on ice that is revealed by many experimental techniques. 1,[34][35][36][37][38][39][40] Other theoretical simulations 41 and surface-sensitive probes 42 observed a very dynamic surface on the (0001) basal plane of hexagonal ice. The larger diffusion coefficients measured in the ultrathin ∼300 Å ice multilayers on Ru(001) may be another indication of a more "fluid-like" layer that enhances diffusion in the near surface region.…”

Section: Discussionmentioning

confidence: 99%

Diffusion of HDO into Single-Crystal H₂¹⁶O Ice Multilayers: Comparison with H₂¹⁸O

1997

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The diffusion of HDO into ultrathin single-crystal H2 16O ice multilayers was investigated using a novel combination of laser-induced thermal desorption (LITD) probing and isothermal desorption depth-profiling. The single-crystal hexagonal ice multilayers were grown epitaxially on a Ru(001) metal substrate, and the diffusion coefficients were measured perpendicular to the basal (0001) facet. The measured HDO diffusion coefficients ranged from D = (2.2 ± 0.3) × 10-16 to D = (3.9 ± 0.4) × 10-14 cm2/s over the temperature range 153−170 K. Arrhenius analysis of the temperature-dependent diffusion coefficients yielded a diffusion activation energy of E A = 17.0 ± 1.0 kcal/mol and a preexponential factor of D 0 = (4.2 ± 0.8) × 108 cm2/s. The similarity of the diffusion coefficients for HDO and H2 18O indicates that H/D exchange does not contribute significantly to HDO diffusion in ice. The agreement between the diffusion kinetics for HDO and H2 18O argues that the HDO diffusion occurs via a molecular transport mechanism. The large diffusion preexponentials for both HDO and H2 18O diffusion into the ultrathin ice multilayers also suggest that bulk transport properties in ice may be perturbed by close proximity to the ice surface.

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“…A sandwich experiment was devised to demonstrate that the H 2 18 O bulk diffusion measurements were not influenced by a possible liquid-like H 2 O layer on the ice surface. 8,[14][15][16][17][18][19][20] This highly fluid layer is monitored at temperatures near the ice melting point, and some experimental results suggest that this layer may persist at temperatures as low as 113 K. 16 In this experiment, a layer of isotopicallylabeled H 2 18 O was sandwiched between two H 2 16 O multilayers, as represented pictorially in Figure 11a. A 28 BL H 2 16 O multilayer was initially grown at 160 K. Subsequently, 1 BL of H 2 18 O was deposited on top of the 28 BL H 2 16 O multilayer at 130 K. An additional 58 BL H 2 16 O multilayer was then condensed on top of the H 2 18 O bilayer at 130 K to create the sandwich.…”

Section: A Surface Diffusionmentioning

confidence: 99%

“…8,10 The "liquid-like" H 2 O layer is also inferred from ice particle sintering and characterized by a variety of experimental techniques. 8,[14][15][16][17][18][19][20] This highly fluid surface layer is clearly observed at temperatures between 243 and 273 K and is associated with rapid H 2 O surface diffusion. In addition, previous investigations have observed that the formation of microporous or crystalline ice may depend largely on the surface diffusion rate.…”

Section: Introductionmentioning

confidence: 99%

Surface and Bulk Diffusion of H₂¹⁸O on Single-Crystal H₂¹⁶O Ice Multilayers

1996

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The surface and bulk diffusion of H 2 18 O on single-crystal H 2 16 O 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 H 2 18 O surface diffusion on the crystalline ice multilayers were performed using a scanning LITD method with mass spectrometric detection. Using a mask, one bilayer of isotopicallylabeled H 2 18 O was deposited on half of a crystalline H 2 16 O ice multilayer. LITD measurements were then used to scan the coverage profile as a function of diffusion time at 140 K. No H 2 18 O 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 H 2 18 O surface diffusion of D S e 5 × 10 -9 cm 2 /s at 140 K. The lack of measurable surface diffusion may indicate that H 2 18 O is diffusing into the underlying ice multilayer. H 2 O 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 H 2 18 O was deposited on a crystalline H 2 16 O 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 H 2 18 O should desorb from the ice surface in ∼7 s at 160 K. However, H 2 18 O was monitored during the desorption of the entire H 2 16 O ice multilayer. This behavior indicates that H 2 18 O is diffusing readily into the underlying ice multilayer. The bulk diffusion coefficient of H 2 18 O into crystalline ice multilayers of various thicknesses was determined to be D B ) 1.5((0.5) × 10 -15 cm 2 /s at 160 K. Sandwich experiments with stacked multilayers confirmed that H 2 18 O 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 E B ) 16.7 ( 1.6 kcal/mol and a preexponential of D 0 ) 9.7((0.5) × 10 7 cm 2 /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 H 2 O 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.

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Ellipsometric Study of the Ice Surface Structure Just Below the Melting Point

Cited by 9 publications

References 5 publications

Surface States of Charge Carriers and Electrical Properties of the Surface Layer of Ice

Surface States of Charge Carriers and Electrical Properties of the Surface Layer of Ice

Diffusion of HDO into Single-Crystal H₂¹⁶O Ice Multilayers: Comparison with H₂¹⁸O

Surface and Bulk Diffusion of H₂¹⁸O on Single-Crystal H₂¹⁶O Ice Multilayers

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Ellipsometric Study of the Ice Surface Structure Just Below the Melting Point

Cited by 9 publications

References 5 publications

Surface States of Charge Carriers and Electrical Properties of the Surface Layer of Ice

Surface States of Charge Carriers and Electrical Properties of the Surface Layer of Ice

Diffusion of HDO into Single-Crystal H216O Ice Multilayers: Comparison with H218O

Surface and Bulk Diffusion of H218O on Single-Crystal H216O Ice Multilayers

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Diffusion of HDO into Single-Crystal H₂¹⁶O Ice Multilayers: Comparison with H₂¹⁸O

Surface and Bulk Diffusion of H₂¹⁸O on Single-Crystal H₂¹⁶O Ice Multilayers