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At least 73 records · Page 4

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.

Hagen, D. E.↗

S 8 ring content in liquid sulfur determined from x-ray diffraction

The S 8 ring content in liquid sulfur has been determined from the 4.47 Å peak in the x-ray pair distribution function over the temperature range −55 °C –330 °C. This peak represents the characteristic 3rd and 4th nearest atom-atom distances across an S 8 -ring. Three procedures were used to calculate the S 8 -ring fraction; scaling to crystalline β-S, a linear combination fit and a direct integration method. All methods gave similar values, indicating that approximately one third of the S 8 -rings break up upon melting into a distribution of short chains with an average length of 5 ± 2 atoms. Our results contradict established models of low temperature sulfur that indicate below the λ-transition the liquid comprises almost entirely of S8-rings. In addition, we find the S 8 -ring fraction increases to 76 ± 10% at −30 °C in the supercooled liquid, and decreases to 23% ± 3% at 330 °C in the high temperature melt. First principle molecular dynamics calculations confirm the onset of dynamic ring distortion via broad bond angle distributions, associated with the interstitial region between the first and second peaks in the pair distribution function. Our results are consistent with the presence of a propensity of short chains in the low temperature liquid, that are required for the bond switching mechanism responsible for the polymerization process to occur at the λ-transition temperature, T λ .

lambda transition↗

Ubiquitous short-range order in multi-principal element alloys

Recent research in multi-principal element alloys (MPEAs) has increasingly focused on the role of short-range order (SRO) on material performance. However, the mechanisms of SRO formation and its precise control remain elusive, limiting the progress of SRO engineering. Here, leveraging advanced additive manufacturing techniques that produce samples with a wide range of cooling rates (up to 10 7 K s –1 ) and an enhanced semi-quantitative electron microscopy method, we characterize SRO in three CoCrNi-based face-centered-cubic (FCC) MPEAs. Surprisingly, irrespective of the processing and thermal treatment history, all samples exhibit similar levels of SRO. Atomistic simulations reveal that during solidification, prevalent local chemical order arises in the liquid-solid interface (solidification front) even under the extreme cooling rate of 10 11 K s –1 . This phenomenon stems from the swift atomic diffusion in the supercooled liquid, which matches or even surpasses the rate of solidification. Therefore, SRO is an inherent characteristic of most FCC MPEAs, insensitive to variations in cooling rates and even annealing treatments typically available in experiments.

36 MATERIALS SCIENCE↗

Cloud Top Phase Characterization of Extratropical Cyclones over the Northeast and Midwest United States: Results from IMPACTS

Cloud top phase (CTP) impacts cloud albedo and pathways for ice particle nucleation, growth, and fallout within extratropical cyclones. This study uses airborne lidar, radar, and Rapid Refresh analysis data to characterize CTP within extratropical cyclones as a function of cloud top temperature (CTT). During the 2020, 2022, and 2023 Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Snowstorms (IMPACTS) field campaign deployments, the Earth-Resources 2 (ER-2) aircraft flew 26 research flights over the Northeast and Midwest U.S. to sample the cloud tops of a variety of extratropical cyclones. A training dataset was developed to create probabilistic phase classifications based on Cloud Physics Lidar measurements of known ice and liquid clouds. These classifications were then used to quantify dominant CTP in the top 150 m of clouds sampled by the Cloud Physics Lidar in storms during IMPACTS. Case studies are presented illustrating examples of supercooled liquid water at cloud top at different CTT ranges (-3°C -20°C. Liquid-bearing cloud tops were found at CTTs as cold as -37ºC.

Troy J. Zaremba↗

Bond-orientational order in liquid Si

Bond-orientational order in liquid Si via Monte Carlo simulation in conjuncation with empirical two- and three-body potentials of the form proposed by Stillinger and Weber are studied. Bond-orientational order (BOO) is described in terms of combinations of spherical harmonic functions. Liquid Si is found to have pronounced short-range BOO corresponding to l = 3, as expected for a structure with local tetrahedral order. No long-range BOO is found either in the equilibrium or the supercooled liquid. When the three-body potential is artificially removed, the tetrahedral bond-orientation order disappears and the liquid assumes a close-packed structure.

Wang, Z. Q.↗

The origin of the Stokes–Einstein relation in simple dense liquids

Here, we investigate the origin of the universal relation between structural relaxation and diffusion in simple dense liquids, known as the Stokes–Einstein (SE) relation. The fact that this relation, originally derived from a hydrodynamic model of a macroscopic particle in a viscous medium, can describe the microscopic-scale liquid dynamics still eludes understanding. We introduce a new universal measure of structural relaxation in a system of N identical particles based on an explicit decomposition of the configuration space into N! congruent convex polyhedra. This measure makes it possible to quantify the correlation between two distinct particle configurations in terms of their minimal Euclidean distance, optimized with respect to particle permutations. Using this measure alongside a model of independent random walkers under the single-occupancy constraint, we derive a master equation that quantifies the SE relation. It allows us to demonstrate that the universal relation between structural relaxation and diffusion in simple dense liquids is caused by two conditions: (a) the confinement of the dominant density fluctuations to the first coordination shell, manifested by de Gennes narrowing, and (b) Gaussianity of the diffusion process; the former is shown to be violated in low-density fluids, and the latter is known to be violated in supercooled liquids.

Physics - Condensed matter physics↗

Use of Polarimetric Radar Measurements to Constrain Simulated Convective Cell Evolution: A Pilot Study with Lagrangian Tracking

To probe the potential value of a radar-driven field campaign to constrain simulation of isolated convection subject to a strong aerosol perturbation, convective cells observed by the operational KHGX weather radar in the vicinity of Houston, Texas, are examined individually and statistically. Cells observed in a single case study of onshore flow conditions during July 2013 are first examined and compared with cells in a regional model simulation. Observed and simulated cells are objectively identified and tracked from observed or calculated positive specific differential phase (K(sub DP)) above the melting level, which is related to the presence of supercooled liquid water. Several observed and simulated cells are subjectively selected for further examination. Below the melting level, we compare sequential cross sections of retrieved and simulated raindrop size distribution parameters. Above the melting level, we examine time series of KDP and radar differential reflectivity (Z(sub DR)) statistics from observations and calculated from simulated supercooled rain properties, alongside simulated vertical wind and supercooled rain mixing ratio statistics. Results indicate that the operational weather radar measurements offer multiple constraints on the properties of simulated convective cells, with substantial value added from derived K(sub DP) and retrieved rain properties. The value of collocated three-dimensional lightning mapping array measurements, which are relatively rare in the continental US, supports the choice of Houston as a suitable location for future field studies to improve the simulation and understanding of convective updraft physics. However, rapid evolution of cells between routine volume scans motivates consideration of adaptive scan strategies or radar imaging technologies to amend operational weather radar capabilities. A 3-year climatology of isolated cell tracks, prepared using a more efficient algorithm, yields additional relevant information. Isolated cells are found within the KHGX domain on roughly 40 % of days year-round, with greatest concentration in the northwest quadrant, but roughly 5-fold more cells occur during June through September. During this enhanced occurrence period, the cells initiate following a strong diurnal cycle that peaks in the early afternoon, typically follow a south-to-north flow, and dissipate within 1 h, consistent with the case study examples. Statistics indicate that ∼ 150 isolated cells initiate and dissipate within 70 km of the KHGX radar during the enhanced occurrence period annually, and roughly 10 times as many within 200 km, suitable for multi-instrument Lagrangian observation strategies. In addition to ancillary meteorological and aerosol measurements, robust vertical wind speed retrievals would add substantial value to a radar-driven field campaign.

Fridlind, Ann M.↗

Growth of needle-shaped crystals in the presence of convection

The motion of the freezing front between a needle-shaped crystal and a supercooled liquid is analyzed for situations where there is forced convection aligned with the crystal axis. It is shown that in the absence of capillary effects the shape of the crystal-melt interface is a paraboloid of revolution, similar to that found in situations where diffusion is the sole heat-transfer mechanism. A relation between the supercooling, the product of tip velocity and tip radius, and the strength of the flow is derived which reduces to the well-known Ivantsov theory in the absence of convection.

Saville, D. A.↗

Determining Cloud Thermodynamic Phase from the Polarized Micro Pulse Lidar

A method to distinguish cloud thermodynamic phase from polarized Micro Pulse Lidar (MPL) measurements is described. The method employs a simple enumerative approach to classify cloud layers as either liquid water, ice water, or mixed-phase clouds based on the linear volume depolarization ratio and cloud top temperatures derived from Goddard Earth Observing System, version 5 (GEOS-5) assimilated data. Two years of cloud retrievals from the Micro Pulse Lidar Network (MPLNET) site in Greenbelt, MD are used to evaluate the performance of the algorithm. The fraction of supercooled liquid water in the mixed-phase temperature regime (-37 °C – 0 °C) calculated using MPLNET data is compared to similar calculations made using the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on board the Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite, with reasonable consistency.

Jasper R Lewis↗

Medium-Range Structural Order as the Driver of Activated Dynamics and Complexity Reduction in Glass-Forming Liquids

Here, we analyze in depth the Elastically Collective Nonlinear Langevin Equation theory of activated dynamics in metastable liquids to establish that the predicted inter-relationships between the alpha relaxation time, local cage and collective elastic barriers, dynamic localization length, and shear modulus are causally related within the theory to the medium range order (MRO) static correlation length. The latter grows exponentially with density for metastable hard sphere fluids and as a nonuniversal inverse power law with temperature for supercooled liquids under isobaric conditions. The physical origin of predicted connections between the alpha time and other metrics of cage order and the thermodynamic inverse dimensionless compressibility is fully established. It is discovered that although kinetic constraints from the real space first coordination shell are important for the alpha time, they are of secondary importance compared to the consequences of the more universal MRO correlations in both the modestly and deeply metastable regimes. This understanding sheds new light on the theoretical basis for, and prior successes of, the predictive mapping of chemically complex thermal liquids to effective hard sphere fluids based on matching their dimensionless compressibilities, a scheme we call “complexity reduction”. In essence, the latter is equivalent to the physical requirement that the thermal liquid MRO correlation equals that of its effective hard sphere analog. The mapping alone is shown to provide a remarkable level of quantitative predictive power for the glass transition temperature T g of 21 molecular and polymer liquids. Predictions for the chemically specific absolute magnitude and growth with cooling of the MRO correlation length are obtained and lie in the window of 2–6 nm at T g . Dynamic heterogeneity, elastic facilitation, and beyond pair structure issues are briefly discussed. Future opportunities to theoretically analyze the equilibrated deep glass regime are outlined.

cancer↗

On the Effects of Cloud Water Content on Passive Microwave Snowfall Retrievals

The Bayesian passive microwave retrievals of snowfall often rely on mathematical matching of the observed vectors of brightness temperature with an a priori database of precipitation profiles and their corresponding brightness temperatures. Mathematical proximity does not necessarily lead to consistent retrievals due to limited information content of passive microwave observations. This paper defines imposter (genuine) vectors of brightness temperature as those that are mathematically close but physically inconsistent (consistent) and characterizes them through the Silhouette Coefficient (SC) analysis. The Neyman–Pearson (NP) hypothesis testing is used to separate the imposter and genuine brightness temperatures based on their associated values of cloud ice (IWP) and liquid water path (LWP), given by coincidences of CloudSat Profiling Radar (CPR) and the Global Precipitation Measurement (GPM) Microwave Imager (GMI). The study determines thresholds for IWP and LWP that allow optimal identification of imposter brightness temperatures of non-snowing and snowing clouds, which can mislead the passive microwave retrieval algorithms to falsely detect or miss the snowfall events. It is demonstrated that emission signal of supercooled liquid water in snowing clouds can lead to improved passive microwave retrieval of snowfall and conditioning the retrievals to the cloud IWP and LWP can result in marginal correction of the snowfall detection probability; however, reduce the probability of false alarm by 6%–8% over sea ice and open oceans.

Snowfall↗

Dendritic growth in the presence of convection

The motion of the freezing front between a dendritic crystal and a supercooled liquid is studied using an interface evolution equation derived from a boundary integral transformation of the transient convective-diffusion equation. A new steady-state theory is introduced that incorporates the effects of convection in dendritic growth. It is shown that in the absence of capillary effects the shape of the crystal-melt interface is a paraboloid of revolution, similar to that found in situations where diffusion is the sole heat transfer mechanism. A relation between the supercooling, the product of the tip velocity and tip radius, and the strength of the flow is derived which reduces to the well-known Ivantsov theory in the absence of convection. A non-linear interface-tracking algorithm is developed and used to study the temporal and spatial evolution of the dendritic interface. The important role of capillarity and convection on the interface dynamics is established and the response of the interface to finite amplitude disturbances is examined for the first time. Tip splitting is identified as the dominant destabilization mechanism in the limit of zero surface tension. Finite surface tension leads to interface stabilization, irrespective of the magnitude and structure of the external perturbations. Finally, convection significantly decreases the magnitude of the freezing velocity.

Beaghton, Pantelis John↗

The effect of fluid flow due to the crystal-melt density change on the growth of a parabolic isothermal dendrite

The Ivantsov (1947) analysis of an isolated isothermal dendrite (with zero surface tension) growing into a supercooled liquid is extended to include the effects of the fluid flow due to volume contraction or expansion upon solidification. For an axisymmetric paraboloidal dendrite, an analytic solution to the Navier-Stokes equations is obtained. The magnitude of the flow is proportional to the relative density change epsilon, and the flow becomes negligible far from the surface of the dendrite. The temperature field consistent with this flow can also be found explicitly. The well-known expression that relates the dimensionless supercooling to the Peclet number in the absence of fluid flow is modified for nonzero epsilon, but the effect is of order epsilon and hence is seen to be minor for most values of epsilon and dimensionless supercooling that occur in practice.

Mcfadden, G. B.↗

Polarization Lidar Liquid Cloud Detection Algorithm for Winter Mountain Storms

We have collected an extensive polarization lidar dataset from elevated sites in the Tushar Mountains of Utah in support of winter storm cloud seeding research and experiments. Our truck-mounted ruby lidar collected zenith, dual-polarization lidar data through a roof window equipped with a wiper system to prevent snowfall accumulation. Lidar returns were collected at a rate of one shot every 1 to 5 min during declared storm periods over the 1985 and 1987 mid-Jan. to mid-Mar. Field seasons. The mid-barrier remote sensor field site was located at 2.57 km MSL. Of chief interest to weather modification efforts are the heights of supercooled liquid water (SLW) clouds, which must be known to assess their 'seedability' (i.e., temperature and height suitability for artificially increasing snowfall). We are currently re-examining out entire dataset to determine the climatological properties of SLW clouds in winter storms using an autonomous computer algorithm.

Sassen, Kenneth↗

HCl Vapour Pressures and Reaction Probabilities for ClONO2 + HCl on Liquid H2SO4-HNO3-HCl-H20 Solutions

Henry's Law solubility constants for HCl have been measured for liquid H2SO4-HNO3-HCl-H2O solutions; the results are in good agreement with predictions from published semiempirical models. The ClONO2 + HCl reaction on the surfaces of such solutions with compositions simulating those of stratospheric aerosols has been investigated; as the composition changes following the temperature drop characteristic of the high-latitude stratosphere the reaction probability gamma increases rapidly. Furthermore, the gamma values remain essentially unchanged when HN03 uptake is neglected; the controlling factor appears to be the solubility of HCl. These results corroborate our earlier suggestion that supercooled liquid sulfate aerosols promote chlorine activation at low temperatures as efficiently as solid polar stratospheric cloud particles.

Elrod, M. J.↗

Low-Level Liquid-Bearing Clouds Contribute to Seasonal Lower Atmosphere Stability and Surface Energy Forcing over a High-Mountain Watershed Environment

Measurements of atmospheric structure and surface energy budgets distributed along a high-altitude moun tain watershed environment near Crested Butte, Colorado, from two separate, but coordinated, field campaigns, Surface Atmosphere Integrated field Laboratory (SAIL) and Study of Precipitation, the Lower Atmosphere, and Surface for Hydrometeorology (SPLASH), are analyzed. This study identifies similarities and differences in how clouds influence the radiative budget over one snow-free summer season (2022) and two snow-covered seasons (2021/22; 2022/23) for this alpine location. A relationship between lower-tropospheric stability stratification and longwave radiative flux from the presence or absence of clouds is identified. When low clouds persisted, often with signatures of supercooled liquid in win ter, the lower troposphere experienced weaker stability, while radiatively clear skies that are less likely to be influenced by liquid droplets were associated with appreciably stronger lower-tropospheric stratification. Corresponding surface turbu lent heat fluxes partitioned differently based upon the cloud–stability stratification regime derived from early morning radiosounding profiles. Combined with the differences in the radiative budget largely resulting from dramatic seasonal dif ferences in surface albedo, the lower atmosphere stratification, surface energy budget, and near-surface thermodynamics are shown to be modified by the effective longwave radiative forcing of clouds. The diurnal evolution of thermodynamics and surface energy components varied depending on the early morning stratification state. Thus, the importance of quies cent versus synoptically active large-scale meteorology is hypothesized as a critical forcing for cloud properties and associ ated surface energy budget variations. The physical relationships between clouds, radiation, and stratification can provide a useful suite of metrics for process understanding and to evaluate numerical models in such an undersampled, highly com plex terrain environment.

54 ENVIRONMENTAL SCIENCES↗

166 GHz Ice Scattering Signal in Cold-Season Precipitating Cloud Systems

Surface snowfall can be produced by a variety of forcing mechanisms that are accompanied by different in-cloud physical processes and microphysical composition. For instance, shallow cumuliform snowfall forced by marine cold air outbreaks shows distinct geographic and seasonal signatures and plays in important role in annual snowfall production in many regions worldwide. Coincident CloudSat-CALIPSO observations confirm that oceanic regions exhibiting frequent shallow cumuliform snow are typically composed of mixed-phase cloud and precipitation particles and display passive microwave brightness temperature behavior that is dominated by cloud liquid water emission, while combined Global Precipitation Measurement (GPM) radiometer and surface radar studies of intense shallow cumuliform events indicate significant ice particle scattering signals at the highest GPM radiometer frequencies. Passive microwave imager channels in the 37 to 89 GHz range have long been used to detect precipitation-sized ice particle scattering signatures in clouds. Dual polarization plays an important role in distinguishing between scattering signatures and other background variability. The GPM Microwave Imager (GMI) is the first satellite radiometer to possess dual-polarized channels at 166 GHz. These high-frequency channels are more susceptible to emission and attenuation by cloud liquid water and water vapor than lower-frequency channels, but are also more sensitive to ice scattering. This research studies the ice scattering information contained in the 166 GHz channels compared to the historically used 85/89 GHz channels on previous sensors. A 166 GHz scattering index (SI) will be developed to understand how its correlation with non-precipitating ice scattering at higher altitudes also affects the 166 GHz scattering signature in cold-season precipitating cloud systems. The 166 GHz SI will be used to possibly isolate precipitation scattering signature for different snowfall modes (shallow convective vs. deep stratiform). The supercooled liquid water affecting shallow convective systems and drastically reducing the scattering signal could be detected and quantified, providing additional information for convective snow detection and quantification in solid precipitation retrieval algorithms.

Lisa Milani↗

Impacts of Synoptic-Scale Dynamics on Clouds and Radiation in High Southern Latitudes

High-latitudinal mixed-phase clouds significantly affect Earth's radiative balance. Observations of cloud and radiative properties from two field campaigns in the Southern Ocean and Antarctica were compared with two global climate model simulations. A cyclone compositing method was used to quantify “dynamics-cloud-radiation” relationships relative to the extratropical cyclone centers. Observations show larger asymmetry in cloud and radiative properties between western and eastern sectors at McMurdo compared with Macquarie Island. Most observed quantities at McMurdo are higher in the western (i.e., post-frontal) than the eastern (frontal) sector, including cloud fraction, liquid water path (LWP), net surface shortwave and longwave radiation (SW and LW), except for ice water path (IWP) being higher in the eastern sector. Here, the two models were found to overestimate cloud fraction and LWP at Macquarie Island but underestimate them at McMurdo Station. IWP is consistently underestimated at both locations, both sectors, and in all seasons. Biases of cloud fraction, LWP, and IWP are negatively correlated with SW biases and positively correlated with LW biases. The persistent negative IWP biases may have become one of the leading causes of radiative biases over the high southern latitudes, after correcting the underestimation of supercooled liquid water in the older model versions. By examining multi-scale factors from cloud microphysics to synoptic dynamics, this work will help increase the fidelity of climate simulations in this remote region.

58 GEOSCIENCES↗