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Microgravity Investigation of Supercooled Fragile Liquid Metal Oxides
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Microgravity Investigation of Supercooled Fragile Liquid Metal Oxides
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Slower nucleation kinetics with stirring in a supercooled Zr80Pt20 liquid—Terrestrial and microgravity experiments on the International Space Station
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Mixed-phase clouds and precipitation in Southern Ocean cyclones and cloud systems observed poleward of 64°S by ship-based cloud radar and lidar
Mixed-phase clouds (MPCs), composed of both liquid and ice, are prevalent in Southern Ocean cyclones. A characterisation of these clouds on fine vertical scales is required in order to understand the microphysical processes within these clouds, and for model and satellite evaluations over this region. We investigated three examples of cloud systems collected by ship-mounted remote sensing instruments adjacent to East Antarctica at latitudes between 64°S and 69°S. These cases allow us to examine the properties of mid-level MPCs, with cloud tops between 2 and 6 km. Mid-level MPCs contain multiple layers of supercooled liquid water (SLW) embedded within ice during the passage of cyclones. SLW layers are capped by strong temperature inversions and are observed at temperatures as low as - 31°C. Convective generating cells (GCs) are present inside supercooled liquid-topped mid-level MPCs. The horizontal extent, vertical extent and maximum upward Doppler velocity of these GCs were 0.6 – 3.6 km, 0.7 – 1.0 km and 0.5 – 1.0 m s -1 , respectively, and are consistent with observations from previous lower-latitude studies. Ice precipitation is nearly ubiquitous, except in the thinnest clouds at the trailing end of the observed systems. Seeding of lower SLW layers from above leads to periods with either larger ice particles or greater ice precipitation rates. Additionally, periods of supercooled drizzle lasting up to two hours were observed toward the end of two of the three cyclone systems. This supercooled drizzle turns into predominantly ice precipitation as the result of seeding by ice clouds located above the precipitating SLW layer.
Using Satellite and ARM Observations to Evaluate Cold Air Outbreak Cloud Transitions in E3SM Global Storm‐Resolving Simulations
Abstract This study examines marine boundary layer cloud regime transition during a cold air outbreak (CAO) over the Norwegian Sea, simulated by a global storm‐resolving model (GSRM) known as the Simple Cloud‐Resolving Energy Exascale Earth System Model Atmosphere Model (SCREAM). By selecting observational references based on a combination of large‐scale conditions rather than strict time‐matched comparisons, this study finds that SCREAM qualitatively captures the CAO cloud transition, including boundary layer growth, cloud mesoscale structure, and phase partitioning. SCREAM also accurately locates the greatest ice and liquid in the mesoscale updrafts, however, underestimates supercooled liquid water in cumulus clouds. The model evaluation approach adopted by this study takes advantages of the existing computational‐expensive global simulations of GSRM and the available observations to understand model performance and can be applied to assessments of other cloud regimes in different regions. Such practice provides valuable guidance on the future effort to correct and improve biased model behaviors.
High Energy Density Physics of Inertial Confinement Fusion Ablator Materials
The historic December 5, 2022 experiment at Lawrence Livermore National Lab’s (LLNL) National Ignition Facility (NIF) reached fusion energy ignition for the first time. This is the most important scientific breakthrough of the 21st century paves the way to future clean inertial fusion energy (IFE). The diamond (high density carbon (HDC)) ablator material used in this experiment displays detrimental effects due to the development of hydrodynamic instabilities at the diamond/fuel interface under shock compression. New alternatives to diamond ablators are required to step up the energy yield in ICF experiments. The unique combination of mechanical strength (approaching that of diamond), the ability to accommodate high-Z dopants (in contrast to diamond), and the tunability of the properties (through synthesis material with varying sp 3 content) make amorphous carbon (a-C) a promising material for next-generation IFE ablative capsules. However, despite its critical importance to the IFE program, the behavior of a-C carbon at extreme temperatures and pressures remains largely unexplored. The primary goals of this project were to perform groundbreaking dynamic compression experiments and predictive simulations to uncover the fundamental high-energy-density physics of amorphous carbon. Our goals were (1) to uncover the metastability range of amorphous carbon and probe phase transitions to diamond or metastable supercooled liquid carbon; (2) to acquire high-quality equation of state (EOS) data and develop an experimentally validated EOS from machine-learning MD simulations of the complex states of carbon; and (3) to uncover the complex behavior of carbon liquid in both thermodynamically stable and metastable supercooled states by accessing large areas of carbon phase diagram with amorphous samples with variable sp 3 content. Our proposed experimental program included measurements of equation of state and diffraction measurements using the Omega EP laser at the Laboratory of Laser Energetics at the University of Rochester. The theoretical/simulation program involved the development of machine-learning models of the complex response of amorphous carbon under dynamic compression by performing molecular dynamics simulations at experimental time and length scales using leadership class DOE supercomputers. Simulations guided experiments to observe predicted phenomena and acquire critical experimental data in specific pressure-temperature domains to validate theoretical models. This research delivered fundamental properties of novel amorphous carbon IFE ablator material, including phase diagram and EOS. These results will aid in IFE target design and implosion experiments. A unique combination of predictive simulations and dynamic and static experiments provided a highly inspirational intellectual environment for graduate students and postdocs involved in this project.
Predicting Frigid Mixed-Phase Clouds for Pristine Coastal Antarctica
Supercooled water is common in the clouds near coastal Antarctica and occasionally occurs at temperatures at or below -30°C. Yet the ice physics in most regional and global numerical models will glaciate out these clouds. This presents a challenge for the simulation of highly supercooled clouds that were observed at McMurdo, Antarctica during the Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment (AWARE) project during 2015–2017. The polar optimized version of the Weather Research and Forecasting model (Polar WRF) with the recently developed two-moment P3 microphysics scheme was used to simulate observed supercooled liquid water cases during March and November 2016. Nudging of the simulations to observed rawinsonde profiles and Antarctic automatic weather station observations provided increased realism and much greater cloud water amounts. Furthermore, sensitivity tests that adjust the ice physics for extremely low ice nucleating particle (INP) concentrations decrease cloud ice and increases the cloud liquid water closer to observed amounts. In these tests, a liquid layer near cloud top is simulated, in agreement with observations. Accurate representation of INP concentrations appears to be critical for the simulation of coastal Antarctic clouds.
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.
A modeling examination of cloud seeding conditions under the warmer climate in Utah, USA
Assessment of how the wintertime cloud seeding conditions over Utah's mountains may change provides essential information for the state to work on increasing its snowpack in the warmer climate. Here in this study, data from the National Center for Atmospheric Research's high-resolution, convection-permitting Weather Research and Forecasting model are used to evaluate suitable conditions for wintertime cloud seeding over Utah's mountains, and to estimate future changes to these conditions under a pseudo-global warming scenario. While previous studies have examined historical cloud seeding conditions, this is the first study that explores the impact of future climate change on these conditions. Based on two atmospheric variables commonly used in cloud-seeding operations, i.e. average temperature from the surface to 1 km above ground level (-20 °C≤T≤-6 °C) and vertically integrated supercooled liquid water (SLW > 0.01 mm), Utah's mountains are suitable for seeding more than 20% of the time during winter. A greater rate of suitability exists in the northern and Uinta Mountains. In the warmer climate under a high-emissions scenario, these seeding conditions may wane as the percentage of precipitating clouds suitable for seeding, about 60% under current conditions, would decline to about 40% across the state with significance. This projected decrease is due to rising temperatures and a decreased frequency of precipitation events. These findings imply that climate warming will narrow the window of opportunity for winter cloud seeding operation in Utah.
Integration of Satellite-Derived Cloud Phase, Cloud Top Height, and Liquid Water Path into an Operational Aircraft Icing Nowcasting System
Operational products used by the U.S. Federal Aviation Administration to alert pilots of hazardous icing provide nowcast and short-term forecast estimates of the potential for the presence of supercooled liquid water and supercooled large droplets. The Current Icing Product (CIP) system employs basic satellite-derived information, including a cloud mask and cloud top temperature estimates, together with multiple other data sources to produce a gridded, three-dimensional, hourly depiction of icing probability and severity. Advanced satellite-derived cloud products developed at the NASA Langley Research Center (LaRC) provide a more detailed description of cloud properties (primarily at cloud top) compared to the basic satellite-derived information used currently in CIP. Cloud hydrometeor phase, liquid water path, cloud effective temperature, and cloud top height as estimated by the LaRC algorithms are into the CIP fuzzy logic scheme and a confidence value is determined. Examples of CIP products before and after the integration of the LaRC satellite-derived products will be presented at the conference.
Liquid Structures and Physical Properties -- Ground Based Studies for ISS Experiments
Studies of electrostatically-levitated supercooled liquids have demonstrated strong short- and medium-range ordering in transition metal and alloy liquids, which can influence phase transitions like crystal nucleation and the glass transition. The structure is also related to the liquid properties. Planned ISS experiments will allow a deeper investigation of these results as well as the first investigations of a new type of coupling in crystal nucleation in primary crystallizing liquids, resulting from a linking of the stochastic processes of diffusion with interfacial-attachment. A brief description of the techniques used for ground-based studies and some results relevant to planned ISS investigations are discussed.
A Simple Model of the Energy Threshold for Snowball Chambers
Cloud and bubble chambers have historically been used for particle detection, capitalizing on supersaturation and superheating, respectively. Here, we present new results from a prototype snowball chamber, in which an incoming particle triggers the crystallization of a purified, supercooled liquid. We demonstrate, for the first time, simulation agreement with our first results from 5 years ago: the higher temperature of the freezing of water and significantly shorter time spent supercooled compared to the control in the presence of a Cf-252 fission neutron source. This is accomplished by combining Geant4 modeling of neutron interactions with the Seitz nucleation model used in superheated bubble chambers, including those seeking dark matter. We explore the possible implications of using this new technology for GeV-scale WIMP searches, especially in terms of spin-dependent proton coupling, and report the first supercooling of WbLS (water-based liquid scintillator).
Surface Crystallization of Cloud Droplets: Implications for Climate Change and Ozone Depletion
The process of supercooled liquid water crystallization into ice is still not well understood. Current experimental data on homogeneous freezing rates of ice nucleation in supercooled water droplets show considerable scatter. For example, at -33 C, the reported freezing nucleation rates vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Until now, experimental data on the freezing of supercooled water has been analyzed under the assumption that nucleation of ice took place in the interior volume of a water droplet. Here, the same data is reanalyzed assuming that the nucleation occurred "pseudoheterogeneously" at the air (or oil)-liquid water interface of the droplet. Our analysis suggest that the scatter in the nucleation data can be explained by two main factors. First, the current assumption that nucleation occurs solely inside the volume of a water droplet is incorrect. Second, because the nucleation process most likely occurs on the surface, the rates of nuclei formation could differ vastly when oil or air interfaces are involved. Our results suggest that ice freezing in clouds may initiate on droplet surfaces and such a process can allow for low amounts of liquid water (approx. 0.002 g per cubic meters) to remain supercooled down to -40 C as observed in the atmosphere.
Liquid-Liquid Transition in Water from First Principles
A long-standing question in water research is the possibility that supercooled liquid water can undergo a liquid-liquid phase transition (LLT) into high- and low-density liquids. Here, we used several complementary molecular simulation techniques to evaluate the possibility of an LLT in an ab initio neural network model of water trained on density functional theory calculations with the SCAN exchange correlation functional. We conclusively show the existence of a first-order LLT and an associated critical point in the SCAN description of water, representing the first definitive computational evidence for an LLT in water from first principles.
Metastability and Ostwald step rule in the crystallisation of diamond and graphite from molten carbon
Abstract Experimental challenges in determining the phase diagram of carbon at temperatures and pressures near the graphite-diamond-liquid triple point are often related to the persistence of metastable crystalline or glassy phases, superheated crystals, or supercooled liquids. A deeper understanding of the crystallisation kinetics of diamond and graphite is crucial for effectively interpreting the outcomes of these experiments. Here, we reveal the microscopic mechanisms of diamond and graphite nucleation from liquid carbon through molecular simulations with first-principles machine learning potentials. Our simulations accurately reproduce the experimental phase diagram of carbon near the triple point and show that liquid carbon crystallises spontaneously upon cooling. Metastable graphite crystallises in the domain of diamond thermodynamic stability at pressures above the triple point. Furthermore, whereas diamond crystallises through a classical nucleation pathway, graphite follows a two-step process in which low-density fluctuations forego ordering. Calculations of the nucleation rates of the two competing phases confirm this result and reveal a manifestation of Ostwald’s step rule, where the strong metastability of graphite hinders the transformation to the stable diamond phase. Our results provide a key to interpreting melting and recrystallisation experiments and shed light on nucleation kinetics in polymorphic materials with deep metastable states.
Progress in the Development of Practical Remote Detection of Icing Conditions
The NASA Icing Remote Sensing System (NIRSS) has been under definition and development at NASA Glenn Research Center since 1997. The goal of this development activity is to produce and demonstrate the required sensing and data processing technologies required to accurately remotely detect and measure icing conditions aloft. As part of that effort NASA has teamed with NCAR to develop software to fuse data from multiple instruments into a single detected icing condition product. The multiple instrument approach utilizes a X-band vertical staring radar, a multifrequency microwave, and a lidar ceilometer. The radar data determine cloud boundaries, the radiometer determines the sub-freezing temperature heights and total liquid water content, and the ceilometer refines the lower cloud boundary. Data is post-processed with a LabVIEW program with a resultant supercooled liquid water profile and aircraft hazard depiction. Ground-based, remotely-sensed measurements and in-situ measurements from research aircraft were gathered during the international 2003-2004 Alliance Icing Research Study (AIRS II). Comparisons between the remote sensing system s fused icing product and the aircraft measurements are reviewed here. While there are areas where improvement can be made, the cases examined suggest that the fused sensor remote sensing technique appears to be a valid approach.
Homogeneous condensation - Freezing nucleation rate measurements for small water droplets in an expansion cloud chamber
Experimental data on ice nucleation, presented in an earlier paper, are analyzed to yield information about the homogeneous nucleation rate of ice from supercooled liquid and the heights of energy barriers to that nucleation. The experiment consisted of using an expansion cloud chamber to nucleate from the vapor a cloud of supercooled pure water drops and the observation of the fraction of drops which subsequently froze. The analysis employed standard classical homogeneous nucleation theory. The data are used to extract the first experimental measurement (albeit indirect) of the activation energy for the transfer of a water molecule across the liquid-ice interface at temperatures near -40 C. The results provide further evidence that the local liquid structure becomes more icelike as the temperature is lowered.