Proton anisotropic chemical shift spectra in a single crystal of hexagonal ice
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Magnonic crystals are artificial media in which magnetic properties such as saturation magnetization or relative permeability are periodically modulated in space, allowing for effective control of the magnonic bandstructure by geometrical structuring. From this end, artificial spin ice - arrays of interacting nanomagnets - can be viewed as reprogrammable twodimensional magnonic crystal. Here, we introduce a new kind of bicomponent artificial spin ice that is made of two dissimilar ferromagnetic metals arranged on complementary lattice sites. It is shown that the resonant dynamics can effectively be controlled based on the distinct magnetic properties of the two materials. We use broadband ferromagnetic resonance to measure the spin-wave eigenmodes of the different sublattices. Here, we compare the ferromagnetic resonance spectra of the single component arrays with the spectrum of a bicomponent system that can be interpreted using a superposition principle. Furthermore, we show that the switching behavior of the sublattices affects one another.
Electron diffraction studies of vapor-deposited water ice have characterized the dynamical structural changes during crystallization that affect volatile retention in cometary materials. Crystallization is found to occur by nucleation of small domains, while leaving a significant part of the amorphous material in a slightly more relaxed amorphous state that coexists metastably with cubic crystalline ice. The onset of the amorphous relaxation is prior to crystallization and coincides with the glass transition. Above the glass transition temperature, the crystallization kinetics are consistent with the amorphous solid becoming a "strong" viscous liquid. The amorphous component can effectively retain volatiles during crystallization if the volatile concentration is approximately 10% or less. For higher initial impurity concentrations, a significant amount of impurities is released during crystallization, probably because the impurities are trapped on the surfaces of micropores. A model for crystallization over long timescales is described that can be applied to a wide range of impure water ices under typical astrophysical conditions if the fragility factor D, which describes the viscosity behavior, can be estimated.
Halos at 22 deg from the sun attributed to randomly-orientated, pristine hexagonal crystals are frequently observed through ice clouds. These frequent sightings of halos formed by pristine crystals pose an apparent inconsistency with the dominance of distorted, nonpristine ice crystals indicated by in situ and remote sensing data. Furthermore, the 46 deg halo, which is associated with pristine hexagonal crystals as well, is observed far less frequently than the 22 deg halo. Considering that plausible mechanisms that could cause crystal distortion such as aggregation, sublimation, riming and collisions are stochastic processes that likely lead to distributions of crystals with varying distortion levels, here the presence of the 22 deg and 46 deg halo features in phase functions of mixtures of pristine and distorted hexagonal ice crystals is examined. We conclude that the 22 deg halo feature is generally present if the contribution by pristine crystals to the total scattering cross section is greater than only about 10% in the case of compact particles or columns, and greater than about 40% for plates. The 46 deg halo feature is present only if the mean distortion level is low and the contribution of pristine crystals to the total scattering cross section is above about 20%, 50% and 70%, in the case of compact crystals, plates and columns, respectively. These results indicate that frequent sightings of 22 deg halos are not inconsistent with the observed dominance of distorted, non-pristine ice crystals. Furthermore, the low mean distortion levels and large contributions by pristine crystals needed to produce the 461 halo features provide a potential explanation of the common sighting of the 22 deg halo without any detectable 46 deg halo.
Abstract Ice-VII is a high-pressure polymorph of H2O ice and an important mineral widely present in many planetary environments, such as in the interiors of large icy planetary bodies, within some cold subducted slabs, and in diamonds of deep origin as mineral inclusions. However, its stability at high pressures and high temperatures and thermoelastic properties are still under debate. In this study, we synthesized ice-VII single crystals in externally heated diamond-anvil cells and conducted single-crystal X-ray diffraction experiments up to 78 GPa and 1000 K to revisit the high-pressure and high-temperature phase stability and thermoelastic properties of ice-VII. No obvious unit-cell volume discontinuity or strain anomaly of the high-pressure ice was observed up to the highest achieved pressures and temperatures. The volume-pressure-temperature data were fitted to a high-temperature Birch-Murnaghan equation of state formalism, yielding bulk modulus KT0 = 21.0(4) GPa, its first pressure derivative KT0′ = 4.45(6), dK/dT = –0.009(4) GPa/K, and thermal expansion relation αT = 15(5) × 10–5 + 15(8) × 10–8 × (T – 300) K–1. The determined phase stability and thermoelastic properties of ice-VII can be used to model the inner structure of icy cosmic bodies. Combined with the thermoelastic properties of diamonds, we can reconstruct the isomeke P-T paths of ice-VII inclusions in diamond from depth, offering clues on the water-rich regions in Earth’s deep mantle and the formation environments of those diamonds.
Artificial spin ices are engineered arrays of dipolarly coupled nanobar magnets. They enable direct investigations of fascinating collective phenomena from their diverse microstates. However, experimental access to ground states in the geometrically frustrated systems has proven difficult, limiting studies and applications of novel properties and functionalities from the low energy states. In this work, we introduce a convenient approach to control the competing diploar interactions between the neighboring nanomagnets, allowing us to tailor the vertex degeneracy of the ground states. We achieve this by tuning the length of selected nanobar magnets in the spin ice lattice. We demonstrate the effectiveness of our method by realizing multiple low energy microstates in a kagome artificial spin ice, particularly the hardly accessible long range ordered ground state—the spin crystal state. Our strategy can be directly applied to other artificial spin systems to achieve exotic phases and explore new emergent collective behaviors.
The process by which liquid cloud droplets homogeneously crystallize into ice is still not well-understood. The ice nucleation process based on the standard and classical theory of homogeneous freezing, initiates within the interior volume of a cloud droplet. Current experimental data on homogeneous freezing rates of ice in droplets of supercooled water, both in air and emulsion oil samples, show considerable scatter. For example, at -33 C, the reported volume-based freezing rates of ice in supercooled water vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Here, we show that the process of ice nucleus formation at the air (or oil)-liquid water interface may help to explain why experimental results on ice nucleation rates yield different results in different ambient phases. Our results also suggest that surface crystallization of ice in cloud droplets can explain why low amounts of supercooled water have been observed in the atmosphere near -40 C.
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Directional solidification of water-based solutions has emerged as a versatile technique to template hierarchical porous materials, but this nonequilibrium process remains incompletely understood. Here, in this study, we use phase-field simulations to shed light on the mechanism that selects the growth direction of the lamellar ice structure that templates those materials. Our results show that this selection can be understood within the general framework of spontaneous parity breaking, yielding quantitative predictions for the tilt angle of lamellae with respect to the thermal axis. The results provide a theoretical basis to interpret a wide range of experimental observations.
Electron paramagetic resonance spectrum of irradiated single crystals of ice at cryogenic temperatures
On Earth, jarosite is a weathering product forming in acidic-oxidative environments from the alteration of iron-bearing minerals in presence of liquid water. Typical settings where this iron-potassium hydrated sulphate is found, are weathering zones of pyrite-rich deposits, evaporative basins and fumaroles. Jarosite is not only known on Earth, it also occurs on Mars, where it has been identified by the Opportunity rover. The mineral was in fact recognized in the finely layered formations outcropping at Meridiani Planum and that were accurately investigated by the rover (Klingelhöfer et al. 2004). Since jarosite requires liquid water to form, its occurrence on Mars has been regarded as an evidence for the occurrence of liquid water in the geologic past of Mars (Elwood-Madden et al., 2004). Since then, many models have been proposed to describe the environments where the precipitation of Martian jarosite took place. The most accepted ones deal with evaporative basins similar to Earth’s playas, others concern volcanic activity and hydrothermal processes. An alternative proposal predicted that jarosite may have formed as a consequence of weathering of mineral dust trapped in massive ice deposits, i.e. the ice-weathering model (Niles & Michalsky, 2009). The hypothesis that jarosite formed on Mars because of low-temperature, acidic and water limited weathering, is not new (Burns, 1987), but until now no direct evidences were available to support it.A potential Earth analogue to investigate such processes is deep Antarctic ice. We present a first investigation of deep ice samples from the Talos Dome ice core (East Antarctica) aimed at the identification of englacial jarosite, so as to support the ice-weathering model. Evidences gathered through independent techniques showed that jarosite is actually present in deep Antarctic ice and results from the weathering of dust trapped into ice. The process is controlled by the re-crystallization of ice grains and the concurrent re-location of impurities at grain-junctions, which both depend on ice depth. This study demonstrates that the deep englacial environment is suitable for jarosite precipitation. Our findings support the hypothesis that, as originally predicted by the ice-weathering model, paleo ice-related processes have been important in thegeologic and geochemical history of Mars.
In the refinement of the crystal structures of ice, the best results obtained so far have been with neutron diffraction because the most troublemaking aspects are the hydrogen atoms. In nine out of twenty ice structures, the hydrogen atoms are disordered, which makes proper refinement more difficult. In our previous paper describing the structure of ice VI we proved that, using Hirshfeld atom refinement (HAR) based on synchrotron X-ray data, it is possible to obtain results comparable with those from neutron experiments. In this work, we investigate another structure of high-pressure disordered ice, cubo-ice (ice VII). Single crystals of cubo-ice were grown under pressure in diamond anvil cells. X-ray diffraction measurements were conducted at a synchrotron source facility (APS, University of Chicago, USA) as well as on our regular in-house laboratory diffractometer with Ag radiation. The data collected were further refined with HAR. Comparison of the structural parameters obtained with those derived from neutron diffraction showed very good agreement in terms of bond lengths and fairly good agreement in terms of hydrogen atom ADPs. We were also able to perform unconstrained refinements with various split-atom models.
The water balance of a hurricane is controlled by boundary layer inflow, near vertical motion in the eyewall causing coalescence precipitation at above and residual ice precipitation at below freezing temperatures, and cirrus outflow at below -40 C aloft. In this paper we address the question of efficiency of water removal by this cirrus outflow which is important for the release of latent heat at high altitudes and its role in the dynamic flow at that level. During NASA's 1998 Convection and Moisture Experiment campaign we acquired microphysical outflow data in order to (1) determine the release and redistribution of latent heat near the top of hurricanes, (2) aid in TRMM algorithm development for remote sensing of precipitation, and (3) determine the optical/radiative characteristics of hurricane outflow. The data were acquired with Particle Measuring Systems two dimensional imaging spectrometers. On 23 August and again during the hurricane's landfall on 26 August, 1998, the NASA DC-8 aircraft penetrated hurricane 'Bonnie' four times each near 200 hPa pressure altitude. The eye crossing times were determined by (1) zero counts of cloud particles, (2) approximately 5 C increases in static and potential temperatures, and (3) minima in speeds and changes of direction of horizontal winds. The vertical winds showed shear between -6 m per second and +4 m per second and tangential winds approached 30 m per second in the eyewall. The particle volumes in the eyewall (determined by the pixels the particles shadowed in the direction of flight [x-direction] and normally to it by the number of diodes that they shadowed [y-direction]) ranged between 0.5 and 5.0 cubic centimeters per cubic meter. With a particle density near 0.2 g per cubic centimeter (determined from in situ melting and evaporation on a surface collector), the 1.0 g per meter corresponding mass of cloud ice ranged between 0.27 and 2.7 g per kilograms yielding horizontal fluxes between 8.1 and 81 g per square meters per second. The outflow ice was concentrated in crystals of a modal size of 190 micrometers. The particle size distributions were heavily skewed toward sizes with 98% of all cirrus particles smaller than the modal size comprising, however, only 20% of the mass. Thus the smaller than modal size particles dominantly affected the optical/radiative characteristics of the cloud, whereas the larger than modal size crystals determined the ice mass, hence dominated latent heating. Questions to be addressed relate to the origin of individual ice particles as the hurricane evolved and the likelihood of pristine and aggregate particle formation under the complicated conditions of rotation and outflow in the eyewall.
Over the past two decades, detailed computational simulations of the intricate three dimensional structures of ice-phase crystals and aggregates of those crystals have been developed. The microwave single-scattering properties of these simulated ice particles have been computed and used to improve quantitative estimates of snow rates and to better deRne the vertical structure of snow water contents in deep convective systems, as derived from satellite-borne passive microwave and/or radar remote sensing measurements. The same icephase particles have more recently been used as the starting point for simulations of melting precipitation using computational melting methods. In the current study, a heuristic melting method, as well as a physically-based melting procedure based on smoothed-particle hydrodynamics, are applied to ice particle models to describe the full evolution of the particles from dry snow to liquid drops. The discrete dipole approximation is utilized to calculate the single-scattering properties of the mixed-phase particles throughout the melting process. Then, the properties of the particles are “mapped” into simpliRed microphysical simulations of particle size spectra in the melting layers of stratiform, precipitating clouds. The bulk single-scattering properties of the melting layers and the sensitivity of their properties to modeling assumptions are explored, and the implications for combined radar-radiometer precipitation remote sensing from GPM are discussed.
In the Arctic, during polar night and early spring, ice clouds are separated into two leading types of ice clouds (TICs): (1) TIC1 clouds characterized by a large concentration of very small crystals and TIC2 clouds characterized by a low concentration of large ice crystals. Using a suitable parameterization of heterogeneous ice nucleation is essential for properly representing ice clouds in meteorological and climate models and subsequently understanding their interactions with aerosols and radiation. Here, we describe a new parameterization for ice crystal formation by heterogeneous nucleation in water-subsaturated conditions coupled to aerosol chemistry in the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). The parameterization is implemented in the Milbrandt and Yau (2005a, b) two-moment cloud microphysics scheme, and we assess how the WRF-Chem model responds to the run-time interaction between chemistry and the new parameterization. Well-documented reference cases provided us with in situ data from the spring 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) over Alaska. Our analysis reveals that the new parameterization clearly improves the representation of the ice water content (IWC) in polluted or unpolluted air masses and shows the poor performance of the reference parameterization in representing ice clouds with low IWC. The new parameterization is able to represent TIC1 and TIC2 microphysical characteristics at the top of the clouds, where heterogenous ice nucleation is most likely occurring, even with the known bias of simulated aerosols by WRF-Chem over the Arctic.
The causes of the charge polarity on the blizzard, which consisted of fractured snow crystals and ice particles, were investigated. As a result, the charging phenomena showed that the characteristics of the blizzard are as follows: (1) In the case of the blizzard with snowfall, the fractured snow particles drifting near the surface of snow field (lower area: height 0.3 m) had positive charge, while those drifting at higher area (height 2 m) from the surface of snow field had negative charge. However, during the series of blizzards two kinds of particles positively and negatively charged were collected in equal amounts in a Faraday Cage. It may be considered that snow crystals with electrically neutral properties were separated into two kinds of snow flakes (charged positively and negatively) by destruction of the snow crystals. (2) In the case of the blizzard which consisted of irregularly formed ice drops (generated by peeling off the hardened snow field), the charge polarity of these ice drops salting over the snow field was particularly controlled by the crystallographic characteristics of the surface of the snow field hardened by the powerful wind pressure.
Pyrocumulus clouds above three Colorado wildfires (Hewlett Gulch, High Park, and Waldo Canyon; all occurred during summer 2012) electrified and produced small intracloud discharges whenever the smoke plumes grew to high altitudes (over 10 km above mean sea level, or MSL). This occurred during periods of rapid wildfire growth, as indicated by the shortwave infrared channel on a geostationary satellite, as well as by incident reports. In the Hewlett Gulch case, the fire growth led to increased updrafts within the plume, as inferred by multiple‐ Doppler radar syntheses, which led to the vertical development and subsequent electrification ‐ a life cycle as short as 30 minutes. The lightning, detected by a threedimensional lightning mapping network, was favored in high‐altitude regions (~10 km MSL) containing modest reflectivities (25 dBZ and lower), ~0 dB differential reflectivity, and reduced correlation coefficient (~0.6‐0.7). This indicated the likely presence of ice particles (crystals and aggregates, possibly rimed) mixed with ash. Though neither multiple‐Doppler nor polarimetric observations were available during the electrification of the High Park and Waldo Canyon plumes, their NEXRAD observations showed reflectivity structures consistent with Hewlett Gulch. In addition, polarimetric and multiple‐Doppler scanning of unelectrified High Park plumes indicated only irregularly shaped ash, and not ice, was present (i.e., reflectivities < 25 dBZ, differential reflectivity > 5 dB, correlation < 0.4), and there was no broaching of the 10 km altitude. Based on these results, the electrification likely was caused by ice‐based processes that did not involve significant amounts of graupel. The results demonstrate the scientific value of multiple‐Doppler and polarimetric radar observations of wildfire smoke plumes ‐ including the ability to distinguish between regions of pure hydrometeors, regions of pure ash, and mixtures of both ‐ and also suggest a possible new application for lightning data in monitoring wildfires.
The electrification (or lack thereof) of pyrocumulus clouds is examined for several different wildfires that occurred during 2012‐2013. For example, pyrocumulus clouds above three Colorado wildfires (Hewlett Gulch, High Park, and Waldo Canyon; all occurred during summer 2012) electrified and produced small intracloud discharges whenever the smoke plumes grew to high altitudes (over 10 km above mean sea level, or MSL). This occurred during periods of rapid wildfire growth, as indicated by the shortwave infrared channel on a geostationary satellite, as well as by incident reports. In the Hewlett Gulch case, the fire growth led to increased updrafts within the plume, as inferred by multiple‐Doppler radar syntheses, which led to the vertical development and subsequent electrification ‐ a life cycle as short as 30 minutes. The lightning, detected by a three‐dimensional lightning mapping network, was favored in high‐altitude regions (~10 km MSL) containing modest reflectivities (25 dBZ and lower), ~0 dB differential reflectivity, and reduced correlation coefficient (~0.6‐0.7). This indicated the likely presence of ice particles (crystals and aggregates, possibly rimed) mixed with ash. Though neither multiple‐Doppler nor polarimetric observations were available during the electrification of the High Park and Waldo Canyon plumes, their NEXRAD observations showed reflectivity structures consistent with Hewlett Gulch. In addition, polarimetric and multiple‐Doppler scanning of unelectrified High Park plumes indicated only irregularly shaped ash, and not ice, was present (i.e., reflectivities < 25 dBZ, differential reflectivity > 5 dB, correlation < 0.4), and there was no broaching of the 10 km altitude. Based on these results, the electrification likely was caused by ice‐based processes that did not involve significant amounts of graupel. Results for pyrocumulus clouds above notable 2013 wildfires that also experienced rapid growth (e.g., Black Forest, Yarnell Hill, West Fork, Tres Lagunas, etc.) will be compared against the 2012 cases, with special emphasis on polarimetric NEXRAD and available lightning measurements, in order to better understand the physical processes responsible for pyrocumulus electrification.