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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

MOSAiC studies of long-lasting mixed-phase cloud events and analysis of the liquid-phase properties of Arctic clouds

Vertically resolved observations of the temporal evolution of mixed-phase clouds (MPCs) were performed over the central Arctic during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, which lasted from October 2019 to September 2020. The research icebreaker Polarstern , drifting with the pack ice for more than 7 months, mostly at latitudes > 85° N, served as a platform for state-of-the-art remote sensing of aerosols and clouds. The use of the recently introduced dual field-of-view (FOV) polarization lidar technique in combination with the well-established lidar-radar retrieval technique provided, for the first time, a robust instrumental basis to monitor the evolution of the liquid and the ice phase of MPCs and the interplay between the two phases. Two long-lasting Arctic MPC events observed close to the North Pole in mid-winter (December 2019) and late summer (September 2020) are discussed to provide new insight into Arctic MPC evolution processes. In the second part of the article, cloud statistics, covering all seasons of a year, are presented. The focus is on the optical and microphysical properties of the liquid phase. These results are solely derived from the dual-FOV lidar observations. The key findings of the study can be summarized as follows: persistent activation of aerosol particles to form water droplets is of great importance for the longevity of MPCs. The observations confirm that ice formation occurs predominantly via immersion freezing. The field studies suggest that the free tropospheric reservoirs of cloud condensation nuclei (CCN) and of ice-nucleating particles (INPs) were always well filled, i.e., the clouds did not exhaust their supply of activatable and activated particles. The observation of long-lasting MPC events, low ice production rates, and a sufficiently large INP reservoir leads to the recommendation to use a time-dependent immersion freezing parameterization in MPC modeling efforts.

Jimenez, Cristofer [Leibniz Inst. for Tropospheric↗
DOE OSTI2023

Phase imaging of irradiated foils at the OMEGA EP facility using phase-stepping X-ray Talbot–Lau deflectometry

Abstract Diagnosing the evolution of laser-generated high energy density (HED) systems is fundamental to develop a correct understanding of the behavior of matter under extreme conditions. Talbot–Lau interferometry constitutes a promising tool, since it permits simultaneous single-shot X-ray radiography and phase-contrast imaging of dense plasmas. We present the results of an experiment at OMEGA EP that aims to probe the ablation front of a laser-irradiated foil using a Talbot–Lau X-ray interferometer. A polystyrene (CH) foil was irradiated by a laser of 133 J, 1 ns and probed with 8 keV laser-produced backlighter radiation from Cu foils driven by a short-pulse laser (153 J, 11 ps). The ablation front interferograms were processed in combination with a set of reference images obtained ex situ using phase-stepping. We managed to obtain attenuation and phase-shift images of a laser-irradiated foil for electron densities above ${10}^{22}\;{\mathrm{cm}}^{-3}$ . These results showcase the capabilities of Talbot–Lau X-ray diagnostic methods to diagnose HED laser-generated plasmas through high-resolution imaging.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Phase Transitions in Metal–Organic Frameworks Directly Monitored through In Situ Variable Temperature Liquid-Cell Transmission Electron Microscopy and In Situ X-ray Diffraction

Zr 6 -based metal–organic frameworks (MOFs) with tetratopic organic linkers have been extensively investigated owing to their versatile structural tunability. While diverse topologies and polymorphism in the resulting MOFs are often encountered with tetratopic linkers and Zr 6 nodes, reports on phase transitions within these systems are rare. Thus, we have a limited understanding of polymorph transformations, hindering the rational development of pure phase materials. In this study, a phase transition from a microporous MOF, scu-NU-906, to a mesoporous MOF, csq-NU-1008, was discovered and monitored through in situ variable temperature liquid-cell transmission electron microscopy (VT-LCTEM), high-resolution transmission electron microscopy (HRTEM), and in situ variable temperature powder X-ray diffraction (VT-PXRD). Furthermore, it was found that the microporous- to-mesoporous transformation in the presence of formic acid occurs via a concomitant dissolution–reprecipitation process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Nucleation and growth of blue phase liquid crystals on chemically-patterned surfaces: a surface anchoring assisted blue phase correlation length

In condensed matter, the correlation length is an essential parameter which describes the distance over which a material maintains its structural properties. In liquid crystals, for the orientational order parameter this characteristic length is of the order of nanometers, while in solid crystals it can extend to macroscopic length scales. Here, we report the measurement of the correlation length, or persistence length, of the crystallographic orientation of blue phases (BPs)—chiral liquid crystals with long-range 3D-crystalline structures and submicron-sized lattice-parameters. These materials exhibit phase transformations that have been identified as the liquid analog of crystal-crystal martensitic transformations. In this work, we use liquid epitaxial growth to achieve spontaneous BP-crystal nucleation and subsequent growth. Specifically, we design patterned substrates made of a binary array of regions with different liquid crystal anchoring, which facilitate a uniform nucleation and growth of BP-crystals with (100)-lattice orientation and a simple cubic symmetry. Furthermore, our results indicate that this simple cubic BP, the so-called blue phase II (BPII), forms first on the patterned surface, thereby propagating the growth of domains in directions parallel or perpendicular to the patterned regions. These results are used to understand the emergence of a surface anchoring assisted BPII-correlation length, taken as the distance over which the BP preserves its lattice orientation, as a function of time and pattern characteristics. We found that BPII single crystals can be achieved on patterned regions whose lateral dimensions are equal to or larger than 10 μm, consistent with our measurements of the BPII-correlation length. This newly acquired understanding of the role of surfaces on the formation of BPs is then used to design processes that permit formation of macroscopically large mono-domain, single-crystal BPs by relying on significantly reduced patterned areas (only part of the area is patterned), a feature that could benefit the applications of this intriguing class of materials.

correlation length↗
DOE OSTI2023

Molecular dynamics analysis of particle number fluctuations in the mixed phase of a first-order phase transition

Molecular dynamics simulations are performed for a finite nonrelativistic system of particles with Lennard-Jones potential. We study the effect of liquid-gas mixed phase on particle number fluctuations in coordinate subspace. A metastable region of the mixed phase, the so-called nucleation region, is analyzed in terms of a noninteracting cluster model. Large fluctuations due to spinodal decomposition are observed. They arise due to the interplay between the size of the acceptance region and that of the liquid phase. These effects are studied with a simple geometric model. The model results for the scaled variance of particle number distribution are compared with those obtained from the direct molecular dynamic simulations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Flow Loop Study of ECT-Based Volume Fraction Monitoring in Oil–Water Two-Phase Flows

Measurement of phase volume fractions in water-containing multiphase flows is necessary for the optimization of a host of industrial flow processes. Many water-containing multiphase flows can be classified as either water-dispersed or water-continuous mixtures. A recently developed approach based on Hanai’s mixture formula and utilizing electrical capacitance tomography (ECT) sensors have shown good potential for obtaining water volume fraction estimates in two-phase water-containing flows with different water salinity levels. However, the proposed approach was investigated via controlled experiments restricted to static configurations while, in practice, multiphase flows can be dynamic and unpredictable. In this work, we perform a flow loop study of the proposed ECT-based method for volume fraction estimation in oil–water two-phase flows. Here, we evaluate the performance of the proposed method in both water-dispersed and water-continuous flow regimes by employing different types of capacitive sensors in cylindrical arrangements and parallel-plate rectangular arrangements.

02 PETROLEUM↗
DOE OSTI2020

Phased: Phase-Aware Submodularity-Based Energy Disaggregation

Energy disaggregation is the task of discerning the energy consumption of individual appliances from aggregated measurements, which holds promise for understanding and reducing energy usage. In this paper, we propose PHASED, an optimization approach for energy disaggregation that has two key features: PHASED (i) exploits the structure of power distribution systems to make use of readily available measurements that are neglected by existing methods, and (ii) poses the problem as a minimization of a difference of sub-modular functions. We leverage this form by applying a discrete optimization variant of the majorization-minimization algorithm to iteratively minimize a sequence of global upper bounds of the cost function to obtain high-quality approximate solutions. PHASED improves the disaggregation accuracy of state-of-the-art models by up to 61% and achieves better prediction on heavy load appliances.

ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION↗
DOE OSTI2020

Structural Manipulation of Phase Transitions by Self‐Induced Strain in Geometrically Confined Thin Films

Strain engineering is a well-known method often used to tune material properties in thin films. The most studied sources of strain are lattice mismatch and differential thermal contraction between the substrate and film. However, in materials which undergo a structural phase transition (SPT), a third and often overlooked source of strain may play a very significant role. If the substrate confines the area of the film, the SPT may induce stress which changes the evolution of the transition. This is a 2D analog of the isochoric phase transition between water and ice, where the freezing point drops below 0 °C. To illustrate this, the prototypical Mott insulator V 2 O 3 which has an SPT coupled to a metal–insulator transition is used to show how self-induced strain can drastically alter structural and electronic properties. This effect provides an elegant approach for mapping the phase diagram of the SPT and the transitions coupled to it. Moreover, the magnitude of self-straining is tunable by modifying the substrate morphology. Furthermore, this effect may be important for numerous materials which exhibit an SPT and are subjected to geometrical constraints.

Kalcheim, Yoav↗
DOE OSTI2022

Effects of composition and canister centerline cooling on microstructure, phase distribution, and chemical durability of dehalogenated iron phosphate waste forms

This paper discusses the effects of composition and canister centerline cooling (CCC) on the microstructures, phase distribution, and chemical durability of dehalogenated iron phosphate waste forms starting from chloride-based salt simulants including KCl (Simple-1), NdCl3 (Simple-2), SrCl2 (Simple-3), LaCl3 (Simple-4), LiCl (Simple-5), CsCl (Simple-6), as well as a complex simulant containing LiCl, KCl, NaCl, CsI, SrCl2, CeCl3, and NdCl3 called ERV2. The simulants represent salt constituents present in salt wastes from electrorefiners used for electrochemical reprocessing. These salts are reacted with ammonium dihydrogen phosphate (ADP) resulting in a NH4Cl (dechlorination) byproduct that is captured and phosphate product containing oxides of the salt cations. This product is further stabilized using Fe2O3 through vitrification at higher temperatures. The results presented herein describe the properties of CCC-treated materials following dechlorination and vitrification including phase identification and quantification, elemental distributions, and chemical durabilities. The chemical durability in the CCC-cooled samples are lower durability than quenched materials for the ERV2 samples. The phases formed upon CCC cooling are very complex compositionally and microstructurally.

iron phosphate glass, iron phosphate waste forms, ↗
DOE OSTI2020

Defect cluster and nonequilibrium gas bubble associated growth in irradiated UMo fuels – a cluster dynamics and phase field model

Irradiation examination shows that gas bubble swelling kinetics is much faster after irradiation-induced recrystallization than that prior recrystallization in UMo fuels. It implies that gas bubbles in coarse grains and small recrystallized grains have different growth behavior. In this work, a phase-field model of gas bubble evolution integrating microstructure dependent cluster dynamics has been developed, for the first time, to study the gas bubble swelling behavior in the recrystallization zone of UMo fuels. Generation, diffusion, reaction, sink, emission and clustering of vacancies and interstitials are described by the cluster dynamics model while a phase-field model is used to describe the evolution of non-equilibrium gas bubbles including nucleation and growth. With the coupled model, the effect of defect generation rate, clustering rate, interstitial emission and sink rates on grain boundaries on the gas bubble evolution are systematically simulated. A set of model parameters (defect generation rate, clustering rate, interstitial emission and sink rates) is determined by comparing measured and simulated gas bubble swelling kinetics. The results demonstrate that interstitial clustering is one of the important physical mechanisms which results in a fast gas bubble swelling kinetics in the recrystallization zone. The developed model can also be extended to study the associated growth of defect and second phase precipitates often observed in irradiated materials.

Hu, Shenyang↗
DOE OSTI2021

From Three-Dimensional Clathrates to Two-Dimensional Zintl Phases AMSb 2 (A = Rb, Cs; M = Ga, In) Composed of Pentagonal M–Sb Rings

Three new antimonide Zintl phases, RbGaSb 2 , CsGaSb 2 , and CsInSb 2 , were discovered during exploration of corresponding A–M–Sb (A = Rb, Cs; M = Ga, In) ternary systems while searching for new clathrates. The AGaSb 2 phases crystallize in the tetragonal space group P4 2 /nmc (No. 137) in the LiBS 2 structure type, while CsInSb 2 crystallizes in lower symmetry in the orthorhombic space group Cmce (No. 64) in the KGaSb 2 structure type with additional disorder of one of the Cs sites. The crystal structures of all three reported AMSb 2 compounds are composed of two-dimensional [MSb 2 ] – tetrahedral layers separated by Rb + or Cs + cations. [MSb 2 ] – layers are built from fused M–Sb pentagons and hexagons, which are also the main structural units for A 8 M 27 Sb 19 clathrate cages. The semiconductor nature of AMSb 2 was suggested by band structure calculations and confirmed by transport property characterization. CsGaSb 2 is a rare example of an n-type pnictide Zintl phase. Finally, all reported compounds exhibit low thermal conductivity typical for complex antimonides of heavy elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Nonadiabatic Dynamics in a Continuous Circularly Polarized Laser Field with Floquet Phase-Space Surface Hopping

Non-adiabatic chemical reactions involving continuous circularly polarized light (cw CPL) have not attracted as much attention as dynamics in unpolarized/linearly polarized light. However, including circularly (in contrast to linearly) polarized light allows one to effectively introduce a complex-valued time-dependent Hamiltonian, which offers a new path for control or exploration through the introduction of Berry forces. Here, we investigate several inexpensive semiclassical approaches for modeling such nonadiabatic dynamics in the presence of a time-dependent complex-valued Hamiltonian, beginning with a straightforward instantaneous adiabatic fewest-switches surface hopping (IA-FSSH) approach (where the electronic states depend on position and time), continuing to a standard Floquet fewest switches surface hopping (F-FSSH) approach (where the electronic states depend on position and frequency), and ending with an exotic Floquet phase-space surface hopping (F-PSSH) approach (wherethe electronic states depend on position, frequency, and momentum). Using a set of model systems with time-dependent complex-valued Hamiltonians, we show that the Floquet phase- space adiabats are the optimal choice of basis as far as accounting for Berry phase effects and delivering accuracy. Furthermore, the F-PSSH algorithm sets the stage for modeling nonadiabatic dynamics under strong externally pumped circular polarization in the future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗