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Surface Crystallization of Supercooled Water in Clouds

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.

Tabazadeh, Azadeh

In-situ High-energy X-ray Diffraction Study of the Local Structure of Supercooled Liquid Si

While changes in the coordination number for liquid silicon upon supercooling, signaling an underlying liquid-liquid phase transition, have been predicted, x-ray and neutron measurements have produced conflicting reports. In particular some studies have found an increase in the first shell coordination as temperature decreases in the supercooled regime, while others have reported increases in the coordination number with decreasing temperature. Employing the technique of electrostatic levitation coupled with high energy x-ray diffraction (125 keV), and rapid data acquisition (100ms collection times) using an area detector, we have obtained high quality structural data more deeply into the supercooled regime than has been possible before. No change in coordination number is observed in this temperature region, calling into question previous experimental claims of structural evidence for the existence of a liquid-liquid phase transition.

Lee, G. W.

Observational Constraint on A Feedback From Supercooled Clouds Reduces Projected Warming Uncertainty

The increase of carbon-dioxide-doubling-induced warming (climate sensitivity) in the latest climate models is primarily attributed to a larger extratropical cloud feedback. This is thought to be partly driven by a greater ratio of supercooled liquid-phase clouds to all clouds, termed liquid phase ratio. We use an instrument simulator approach to show that this ratio has increased in the latest climate models and is overestimated rather than underestimated as previously thought. In our analysis of multiple models, a greater ratio corresponds to stronger negative cloud feedback, in contradiction with single-model-based studies. We trace this unexpected result to a cloud feedback involving a shift from supercooled to warm clouds as climate warms, which corresponds to greater cloud amount and optical depth and weakens the extratropical cloud feedback. Better constraining this ratio in climate models – and thus this supercooled cloud feedback – impacts their climate sensitivities by up to 1 ˚C and reduces inter-model spread.

Climate and Earth system modelling

Experimental Study of Supercooled Large Droplet Impingement Effects

Typically, ice accretion results from small supercooled droplets (droplets cooled below freezing), usually 5 to 50 microns in diameter, which can freeze upon impact with an aircraft surface. Recently, ice accretions resulting from supercooled large droplet (SLD) conditions have become a safety concern. Current ice accretion codes have been extensively tested for Title 14 Code of Federal Regulations Part 25, Appendix C icing conditions but have not been validated for SLD icing conditions. This report presents experimental methods for investigating large droplet impingement dynamics and for obtaining small and large water droplet impingement data.

ICE ACCRETION CODE

Supercooled phase transitions in conformal dark sectors explain NANOGrav data

According to recent lore, it is difficult to explain the evidence for a stochastic gravitational wave background obtained by pulsar timing arrays with supercooled first-order phase transitions (FOPTs). We demonstrate that supercooled FOPTs in dark U(1) models with a conformal dark sector easily explain the nHz signal at NANOGrav.

Conformal models

X-ray diffraction of metastable structures from supercooled liquid hydrogen

We report time resolved observations of the crystallization from liquid hydrogen, supercooled to temperatures below the melting point, using 11.2 keV X-ray diffraction from the Linac Coherent Light Source (LCLS). Changes to the metastable solid and liquid structure factors have been dynamically measured. This allows for a direct determination of the lowest energy crystal polymorphs, the stacking probabilities, as well as the liquid and solid densities and temperatures. Such measurements provide experimental evidence of an Arrhenius-like growth kinetics along the stacking direction during supercooling.

36 MATERIALS SCIENCE

Emergent facilitation and glassy dynamics in supercooled liquids

In supercooled liquids, dynamical facilitation refers to a phenomenon where microscopic motion begets further motion nearby, resulting in spatially heterogeneous dynamics. This is central to the glassy relaxation dynamics of such liquids, which show super-Arrhenius growth of relaxation timescales with decreasing temperature. Despite the importance of dynamical facilitation, there is no theoretical understanding of how facilitation emerges and impacts relaxation dynamics. Here, we present a theory that explains the microscopic origins of dynamical facilitation. We show that dynamics proceeds by localized bond-exchange events, also known as excitations, resulting in the accumulation of elastic stresses with which new excitations can interact. At low temperatures, these elastic interactions dominate and facilitate the creation of new excitations near prior excitations. Using the theory of linear elasticity and Markov processes, we simulate a model, which reproduces multiple aspects of glassy dynamics observed in experiments and molecular simulations, including the stretched exponential decay of relaxation functions, the super-Arrhenius behavior of relaxation timescales as well as their two-dimensional finite-size effects. The model also predicts the subdiffusive behavior of the mean squared displacement (MSD) on short, intermediate timescales. Furthermore, we derive the phonon contributions to diffusion and relaxation, which when combined with the excitation contributions produce the two-step relaxation processes, and the ballistic–subdiffusive–diffusive crossover MSD behaviors commonly found in supercooled liquids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Profiling Supercooled Liquid Water Clouds with Multi-Frequency Radar

An optimal estimation scheme is employed to demonstrate the utility of using multi-band radar observations for estimating supercooled liquid profiles. Qualitative comparisons with microphysical probe images show that the retrievals are capable of producing supercooled liquid consistent with in situ data. Finally, a path forward for quantifying performance and extending the study to a more robust measurement suite is given.

supercooled liquid

Better Constraining Supercooled Clouds Could Reduce Projected Warming Spread

The increase of climate sensitivity to rising greenhouse gas concentrations in the coupled model intercomparison project phase 6 (CMIP6) Earth system models (ESMs) compared to CMIP5 ESMs is primarily attributed to a larger extratropical cloud response to climate change, referred to as cloud feedback. The ratio of supercooled liquid cloud water relative to all cloud water, termed liquid phase ratio (LPR), which has also notably increased in many recent ESMs, is thought to be a primary driver of the extratropical cloud feedback increase. Unlike the preponderance of previous studies that compare native model LPR directly with observations, here we evaluate LPR over three ESM generations against Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) using an instrument simulator approach, which mimics instrument limitations and uses consistent cloud definitions and resolutions. We find that current coupled model intercomparison project (CMIP) ESMs collectively simulate greater LPR than previous CMIP generations and overestimate LPR compared to observations, contrary to previous findings, likely driven by past inconsistent comparisons of ESM outputs with CALIPSO observations. We further show that greater LPR in ESM present-day climate is unexpectedly correlated with a smaller extratropical cloud feedback, attributable to a decrease of cloud amount exceeding the increase of cloud optical depth. Finally, our results suggest that improving constraints on model LPR using our evaluation framework would likely reduce the spread in CMIP6 climate sensitivities, owing to its effect on extratropical cloud feedback from supercooled clouds.

greenhouse gas concentrations

Gravitational waves from supercooled phase transitions in conformal Majoron models of neutrino mass

We study supercooled first-order phase transitions above the QCD scale in a wide class of conformal Majoron-like U(1)′ models that explain the totality of active neutrino oscillation data and produce a detectable stochastic gravitational wave background (SGWB) at LIGO, LISA and ET. We place constraints on the U(1)′ breaking scale and gauge coupling using current LIGO-Virgo-Kagra data. We find that strong supercooling can be ruled out in large regions of parameter space if a SGWB is not detected by these experiments. A null signal at LIGO and ET will disfavor a type-I seesaw scale above 10 14 GeV, while a positive signal is a signature of heavy right-handed neutrinos. On the other hand, LISA will be sensitive to seesaw scales as low as a TeV, and could detect a SGWB even if the right-handed neutrinos are decoupled.

early universe particle physics

Supercooling on the lunar surface - A review of analogue information

Terrestrial analog studies of the phase petrology of supercooled melts and rapid crystal growth are reviewed for possible light shed on lunar crystallization, supercooling, and petrogenic processes, in particular rapid consolidation of lavas extruded on the lunar surface, and impact liquids. Crystallization of major constituent minerals (olivine, pyroxene, plagioclase) in dendritic or skeletal forms is found much more characteristic of lunar igneous rocks than of terrestrial counterparts. Olivine and pyroxene occur often as skeletal phenocrysts, and their stage of crystallization is crucial to the genesis and cooling history of porphyritic lavas. Widespread occurrence of glass and of immature radiate crystallization, particularly of highly zoned pyroxenes and zoned plagioclase, is noted.

Donaldson, C. H.

X-Ray Diffraction Study of the Internal Structure of Supercooled Water

A Bragg X-ray spectrometer equipped with a volume-sensitive Geiger counter and Soller slits and employing filtered molybdenum Ka radiation was used to obtain a set of diffracted intensity curves as a Punction of angle for supercooled water. Diffracted intensity curves in the temperature region of 21 to -16 C were obtained. The minimum between the two main diffraction peaks deepened continuously with lowering temperature, indicating a gradual change in the internal structure of the water. No discontinuity in this trend was noted at the melting point. The internal structure of supercooled water was concluded to become progressively more ice-like as the temperature is lowered.

Dorsch, Robert G.

Effects of supercooling in the initial solidification of PbTe-SnTe solid solutions

Deviations from compositions anticipated by the thermal equilibrium phase diagram have been observed in Bridgman-grown crystals of Pb(1-x)Sn(x)Te, in the first to freeze region of the boule. A set of experiments were conducted to determine the extent of thermal supercooling of Pb(1-x)Sn(x)Te in a Bridgman-like configuration. The results of the compositional profiles and the supercooling measurements are consistent with a diffusionless transformation occurring at the onset of solidification, and the length of uncontrolled growth is inversely related to the temperature gradient of the furnace.

Fripp, A. L.

ETO lidar studies of cirrostratus altocumulogenitus: Another role for supercooled liquid water in cirrus cloud formation

Cirrus clouds have traditionally been viewed as cold, wispy, or stratiform ice clouds, typically displaying optical phenomena such as haloes. A composition entirely of hexagonal ice crystals, of one habit or another could only have a transitory existence in cirrus, since the concentrations of ice nuclei (IN) measured by various techniques (at the surface or in the lower troposphere) indicate an enormous number of IN that should be active at cirrus cloud temperatures. In light of recent instrumental aircraft and polarization lidar studies of cirrus clouds, it is clear that highly supercooled cloud droplets can sometimes be a component of cirrus clouds. It remains to be determined if supercooled liquid water (SLW) is present abundantly enough in cirrus to play a significant role in earth's radiance balance, or is merely a curious, infrequent occurrence. To help evaluate this issue, the UH polarization lidar FIRE Extended Time Observation (ETO) of cirrus clouds are being utilized to compile, among other parameters, a climatological record of SLW clouds associated with and within cirrus.

Sassen, Kenneth

The vapor pressures of supercooled NHO3/H2O solutions

A procedure utilizing the Gibbs-Duhem relation is used to extrapolate vapor pressures of supercooled HNO3 mixtures to 190 K. Values of A and B from the equation logP = A - B/T are presented for solutions between 0.20 and 0.25 mole fraction HNO3. In the stratosphere, if sufficient HNO3 vapor is present because it has not come into equilibrium with the nitric acid trihydrate, supercooled nitric acid solutions could condense at temperatures up to 1.5 + or - 0.8 K above the ice point.

Hanson, David R.

NASA/FAA/NCAR Supercooled Large Droplet Icing Flight Research: Summary of Winter 1996-1997 Flight Operations

During the winter of 1996-1997, a flight research program was conducted at the NASA-Lewis Research Center to study the characteristics of Supercooled Large Droplets (SLD) within the Great Lakes region. This flight program was a joint effort between the National Aeronautics and Space Administration (NASA), the National Center for Atmospheric Research (NCAR), and the Federal Aviation Administration (FAA). Based on weather forecasts and real-time in-flight guidance provided by NCAR, the NASA-Lewis Icing Research Aircraft was flown to locations where conditions were believed to be conducive to the formation of Supercooled Large Droplets aloft. Onboard instrumentation was then used to record meteorological, ice accretion, and aero-performance characteristics encountered during the flight. A total of 29 icing research flights were conducted, during which "conventional" small droplet icing, SLD, and mixed phase conditions were encountered aloft. This paper will describe how flight operations were conducted, provide an operational summary of the flights, present selected experimental results from one typical research flight, and conclude with practical "lessons learned" from this first year of operation.

Miller, Dean

Metastable Demixing of Supercooled Cu-Co and Cu-Fe Alloys in an Oxide Flux

A systematic study on the liquid separation in supercooled Cu-Co and Cu-Fe alloys was performed using a melt fluxing which permits high supercooling to be achieved. Moreover, this method renders it possible to directly measure binodal temperatures and establish metastable liquid miscibility gap (LMG). All phase-separated samples at compositions ranging from 10 to 80 wt pct Co or to 83 wt pct Fe were found to exhibit droplet-shaped morphologies, in spite of various droplet distributions. Uniformly dispersed microstructures were obtained as the minority component was less than 20 vol.%; while beyond this percentage, serious coarsening was brought about. Calculations of the miscibility gap in the Cu-Co system and Stokes movement velocity of Co and Fe droplets in Cu matrix were made to analyze the experimental results.

Li, D.

Numerical Analysis Using WRF-SBM for the Cloud Microphysical Structures in the C3VP Field Campaign: Impacts of Supercooled Droplets and Resultant Riming on Snow Microphysics

Two distinct snowfall events are observed over the region near the Great Lakes during 19-23 January 2007 under the intensive measurement campaign of the Canadian CloudSat/CALIPSO validation project (C3VP). These events are numerically investigated using the Weather Research and Forecasting model coupled with a spectral bin microphysics (WRF-SBM) scheme that allows a smooth calculation of riming process by predicting the rimed mass fraction on snow aggregates. The fundamental structures of the observed two snowfall systems are distinctly characterized by a localized intense lake-effect snowstorm in one case and a widely distributed moderate snowfall by the synoptic-scale system in another case. Furthermore, the observed microphysical structures are distinguished by differences in bulk density of solid-phase particles, which are probably linked to the presence or absence of supercooled droplets. The WRF-SBM coupled with Goddard Satellite Data Simulator Unit (G-SDSU) has successfully simulated these distinctive structures in the three-dimensional weather prediction run with a horizontal resolution of 1 km. In particular, riming on snow aggregates by supercooled droplets is considered to be of importance in reproducing the specialized microphysical structures in the case studies. Additional sensitivity tests for the lake-effect snowstorm case are conducted utilizing different planetary boundary layer (PBL) models or the same SBM but without the riming process. The PBL process has a large impact on determining the cloud microphysical structure of the lake-effect snowstorm as well as the surface precipitation pattern, whereas the riming process has little influence on the surface precipitation because of the small height of the system.

lake-effect