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At least 559 records · Page 31

Prognostic model and failure mechanisms of steam generators in Sodium-Cooled fast reactors

This paper presents a prognostic model for sodium-cooled fast reactor (SFR) steam generators (SGs). Here, the purpose of the model is to estimate the remaining useful life of SFR SGs and thus to support the decision-making of autonomous control. SFR SGs are of great interest for plant integrity due to their harsh operation environment. They operate at higher temperatures and higher coolant-to-steam pressure differences than those of current light water reactors (LWR). The severity of the SFR SG failure consequences, which include water-sodium contact, is another reason. Understanding its failure mechanisms is important for the development of its prognostic model. Based on our literature review and physics-based analysis, we concluded that creep would be a dominant degradation mode of SFR SGs due to SFR’s high-temperature and high-pressure environment. Thus, creep is the focus of the prognostic model. Various other failure modes were also investigated in this study. The mechanical fatigue due to flow-induced vibration is usually observed in early developmental phases and would not be an important issue during normal operation. The thermal fatigue due to thermal stripping is occasionally observed in other components in SFRs but does not affect SG integrity. Pure water stress corrosive crack, fretting, and so on are commonly observed in LWR SGs but are significantly less important in SFR SGs because of the high temperatures, high pressure differences, and chemical properties of liquid sodium. Based on these investigations, a prognostic model focusing on creep failures was developed. It estimates the failure probability profile by sampling the Larson-Miller parameter (LMP) and temperature and associated uncertainties through Monte Carlo methods. Two case studies were presented. The first one demonstrated the model’s capability to calculate the failure probability for a new specimen within a given time. If the tube is working under temperatures of 500C ± 3 and pressures of 15.2 MPa, which leads to LMP of 20,100 ± 50, the failure probabilities within 50, 70, and 90 years are approximately 0.1 %, 3.2 %, and 17.5 %. The second demonstrated how adjusting the workload can help to protect the integrity of the component. For an old tube reaching 99 % of its lifespan, continuing to run at temperatures of 500C ± 3 and LMP of 20,100 ± 50 leads to a failure probability of about 29.0 % within a year. If the temperature is reduced by 5C, the failure probability can be reduced to 2.5 %, and, if the pressure is also reduced such that the LMP is increased by 100, the failure probability can further be reduced to 0.12 %.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Semi-solid alkali metal electrodes enabling high critical current densities in solid electrolyte batteries

The need for higher energy density rechargeable batteries has generated interest in alkali metal electrodes paired with solid electrolytes. However, metal penetration and electrolyte fracture at low current densities have emerged as fundamental barriers. Here, we show that for pure metals in the Li-Na-K system, the critical current densities scale inversely to mechanical deformation resistance. Furthermore, we demonstrate two electrode architectures in which the presence of a liquid phase enables high current densities while preserving the shape retention and packaging advantages of solid electrodes. First, biphasic Na-K alloys show K + critical current densities (with K-β*-Al 2 O 3 electrolyte) that exceed 15 mA∙cm -2 . Second, introducing a wetting interfacial film of Na-K liquid between Li metal and Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 (LLZTO) solid electrolyte doubles the critical current density and permits cycling at areal capacities exceeding 3.5 mAh∙cm -2 . These design approaches hold promise for overcoming electro-chemo-mechanical stability issues that have heretofore limited performance of solid-state metal batteries.

25 ENERGY STORAGE↗

Room temperature colossal superparamagnetic order in aminoferrocene–graphene molecular magnets

Intensive studies are published for graphene-based molecular magnets due to their remarkable electric, thermal, and mechanical properties. However, to date, most of all produced molecular magnets are ligand based and subject to challenges regarding the stability of the ligand(s). The lack of long-range coupling limits high operating temperature and leads to a short-range magnetic order. Herein, we introduce an aminoferrocene-based graphene system with room temperature superparamagnetic behavior in the long-range magnetic order that exhibits colossal magnetocrystalline anisotropy of 8 × 10 5 and 3 × 10 7 J/m 3 in aminoferrocene and graphene-based aminoferrocene, respectively. These values are comparable to and even two orders of magnitude larger than pure iron metal. Aminoferrocene [C 10 H 11 FeN] + is synthesized by an electrophilic substitution reaction. It was then reacted with graphene oxide that was prepared by the modified Hammers method. The phase structure and functionalization of surface groups were characterized and confirmed by XRD, FT-IR, and Raman spectroscopy. To model the behavior of the aminoferrocene between two sheets of hydroxylated graphene, we have used density functional theory by placing the aminoferrocene molecule between two highly ordered hydroxylated sheets and allowing the structure to relax. Here, the strong bowing of the isolated graphene sheets suggests that the charge transfer and resulting magnetization could be strongly influenced by pressure effects. In contrast to strategies based on ligands surface attachment, our present work that uses interlayer intercalated aminoferrocene opens routes for future molecular magnets as well as the design of qubit arrays and quantum systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Synthesis and characterization of polylactic acid microspheres via emulsion-based processing

Polylactic acid (PLA) microspheres are primarily used in drug delivery applications and rarely manufactured commercially. In encapsulation, the drug encapsulation and microsphere synthesis process happen simultaneously. Simultaneous synthesis necessitates conditions that ensure the drugs to be encapsulated remain viable in the synthesis process. Here, in the present work, solid pure PLA microspheres are prepared using a repeatable centrifugal mixing method to create a single emulsion system. A planetary thinky mixer is used to achieve centrifugal mixing. PLA acts as the dispersed phase of the emulsion, whereas Polyvinyl alcohol (emulsifier) dissolved in deionized water serves as the bulk phase. The emulsions are stirred for about 4 min at 2000 rpm. Microspheres prepared by mechanical mixing are compared with microspheres prepared by centrifugal mixing. The microspheres prepared by centrifugal mixing proved to be narrower and closer to a normal distribution with a mean size (D x 50) of 30 microns. The size distribution of planetary mixed microspheres did not change from one batch to another.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Using Diffuse Scattering to Observe X-Ray-Driven Nonthermal Melting

We present results from the SPring-8 Angstrom Compact free electron LAser (SACLA) XFEL facility, using a high intensity ($\sim\!10^{20}\,$W/cm$^2$) X-ray pump X-ray probe scheme to observe changes in the ionic structure of silicon induced by X-ray heating of the electrons. By avoiding Laue spots in the scattering signal from a single crystalline sample, we observe a rapid rise in diffuse scattering, which we attribute to a loss of lattice order and a transition to a liquid state within 100 fs of irradiation, a timescale which agrees well with first principles simulations, but is faster than that predicted by purely inertial behavior. This method is capable of observing liquid scattering without masking or filtering of signal from the ambient solid, allowing the liquid structure to be measured throughout and beyond the phase change.

Hartley, Nicholas J.↗

Neutron imaging of hydrogenous gases in porous-carbon materials around phase transitions

Focus herein is on hydrogenous gases interacting with porous-carbon materials on activated biochar at pressures ranging from 0 to 100 bar and temperatures from room (ambient) to cryogenic. Neutron radiography was conducted using a custom-made cell system to simultaneously image pure gas and gas interacting with the porous carbon. From neutron attenuation, the cross sections of methane and ethane and number concentrations were determined for different pressures and temperatures and compared with corresponding reference data. Sorption properties of the porous materials were investigated in situ with methane, ethane, and propane.

Ossler, Frederik [Lund University, Sweden]↗

Dual aggregation steering in bulk-heterojunction via solvent engineering toward efficient and stable binary organic solar cells

In high-performance organic solar cells (OSCs), efficient charge transport hinges on a well-optimized morphology of the photoactive layer, which depends critically on controlled aggregation and favorable interactions between donor and acceptor materials. In this work, we introduce a cascade solvent system comprising high-boiling-point ethylbenzene (EB) and low-boiling-point chloroform (CF) to finely tune the aggregation behavior of the D18 donor and L8-BO acceptor. The incorporation of EB not only promotes the H-aggregation of D18 and the J-aggregation of L8-BO but also facilitates the formation of ideal nanoscale phase separation, thereby suppressing bimolecular recombination. As a result, devices processed with the EB/CF solvent blend achieve a best power conversion efficiency (PCE) of 19.6 % and enhanced operational stability, outperforming those fabricated with pure CF (17.1 %). In conclusion, this study offers a reliable and effective strategy for optimizing donor and acceptor aggregation, providing a viable pathway toward higher-performance OSCs.

36 MATERIALS SCIENCE↗

Three-state Potts nematic order in stacked frustrated spin models with SO(3) symmetry

Here, we propose stacked two-dimensional lattice designs of frustrated and SO(3) symmetric spin models consisting of antiferromagnetic (AF) triangular and ferromagnetic (FM) sixfold symmetric sublattices that realize emergent $\mathbb{Z}_{3}$ Potts nematic order. Considering bilinear-biquadratic spin interactions, our models describe an SO(3)-symmetric triangular lattice AF subject to a fluctuating magnetization arising from the FM coupled sublattice. We focus on the classical AFM-FM windmill model and map out the zero- and finite-temperature phase diagram using Monte Carlo simulations and analytical calculations. We discover a state with composite Potts nematic order above the ferrimagnetic three-sublattice up-up-down ground state and relate it to Potts phases in SO(3)-broken Heisenberg and Ising AFMs in external magnetic fields. Finally, we show that the biquadratic exchange in our model is automatically induced by thermal and quantum fluctuations in the purely bilinear Heisenberg model, easing the requirements for realizing these lattice designs experimentally.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The state of zinc in methanol synthesis over a Zn/ZnO/Cu(211) model catalyst

The active chemical state of zinc (Zn) in a zinc-copper (Zn-Cu) catalyst during carbon dioxide/carbon monoxide (CO 2 /CO) hydrogenation has been debated to be Zn oxide (ZnO) nanoparticles, metallic Zn, or a Zn-Cu surface alloy. We used x-ray photoelectron spectroscopy at 180 to 500 millibar to probe the nature of Zn and reaction intermediates during CO 2 /CO hydrogenation over Zn/ZnO/Cu(211), where the temperature is sufficiently high for the reaction to rapidly turn over, thus creating an almost adsorbate-free surface. Tuning of the grazing incidence angle makes it possible to achieve either surface or bulk sensitivity. Hydrogenation of CO 2 gives preference to ZnO in the form of clusters or nanoparticles, whereas in pure CO a surface Zn-Cu alloy becomes more prominent. Here, the results reveal a specific role of CO in the formation of the Zn-Cu surface alloy as an active phase that facilitates efficient CO 2 methanol synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Report on Depth-Dependent Q from Frequency-Dependent Lg Q

As a phase that travels through the crustal waveguide, Lg samples the velocity and attenuation structure of the crust. We have developed methods (Pasyanos et al., 2009a; Pasyanos et al., 2009b) to estimate Qp and Qs of the crust and upper mantle from the amplitudes of regional phases, and have applied it to a number of regions around the world, and over a broad frequency band (0.5 - 10 Hz). In prior attenuation modeling, Lg phase amplitudes are able to effectively distinguish the high Q (low attenuation) of old stable cratonic crust from the low Q (high attenuation) of more recently active tectonic regions. For a variety of purposes (e.g. waveform modeling, seismic hazard, etc.), it is useful to have more information on the depth-dependence of the Q structure in the crust. One obvious candidate for doing this is using the frequency-dependence information of Lg Q, in the manner of surface waves. Unfortunately, however, Lg samples the whole of the crust without much differentiation with respect to frequency that is characteristic of fundamental mode surface waves. Lg is generally thought to be the sum of supercritically reflected S-waves trapped in the crustal waveguide (e.g. Xie and Lay, 1994). The phase can also be modeled as a superposition of surface waves. At lower frequencies, it is primarily composed of fundamental and low-order surface waves, while at higher frequencies, it is comprised purely of many high-order surface waves. The low-order surface waves that comprise Lg in low frequency bands (< 1 Hz) are preferentially sensitive to shallow earth structure, such as sedimentary basins and upper crust, while high-order surface waves have a more homogenized sensitivity to the whole crust. Furthermore, at the lower frequencies, we might expect to see some differentiation in the sensitivity between early Lg (herein referred to as Lg1) and late Lg (referred to as Lg2) where the latter is comprised of lower-order surface waves and, hence, shallower structure. Therefore, we might expect to see the signature of shallow features, primarily the lower Q of sediments as compared to crystalline crust, at lower frequencies and in later arriving Lg amplitudes.

58 GEOSCIENCES↗

Quantitative characterization of gradient microstructures: A study on friction stir spot processing of pure cobalt

Heterogeneous microstructures in polycrystalline metals can enhance the strength and ductility, outperforming homogeneous structures of similar composition. This study investigates deformed cobalt via friction stir spot processing with varying dwell times to uncover the effects of plastic deformation and heat generation on the formation of morphological, phase, and grain boundary character gradients. A new approach to quantify the morphological gradients in materials, which describes grain morphology in terms of density followed by parametric regression, enables direct quantification of processing depth and gradient sharpness. Results show that longer processing times increase the steepness of morphological gradients and reduce the deformation depth for friction stir spot processing with low plunge depths and high tool rotational speeds. The amount of retained FCC is increased in the shorter processing conditions, primarily due to refined grain size, increased defect content, and reduced heat generation. Crystallographic texture analysis of the HCP phase indicated a dominant B-fiber described by (0001) ∥ shear plane normal in the extreme processing conditions and the formation of a P-fiber, shear direction ∥ ⟨11$\bar2$0⟩ for intermediate dwell times. The texture of the FCC phase for low processing times was a C texture {100}⟨011⟩ where longer processing times were dominated by a [001] fiber texture with a main {110}⟨100⟩ orientation and emergence of a slight [111] fiber in the longest processing condition. The approaches outlined in this work give insight into quantifying gradients and improve the understanding of highly deformed cobalt.

36 MATERIALS SCIENCE↗

Reduced-Order Modeling Method for Phase-Change Thermal Energy Storage Heat Exchangers

Thermal energy storage can facilitate the effective utilization of renewable energy. To speed up the design process of thermal energy storage devices, it is critical to develop fast and accurate modeling methods for phase change material embedded heat exchangers (PCM HXs). This study developed and compared two approximation-assisted reduced-order PCM HX models for the simulation of thermal storage components and systems, which were verified against a validated finite-volume model. They are a pure black-box model, and a grey-box model based on the Number of Transfer Units (or effectiveness-NTU) approach. We used the reduced-order models to predict the performance of standalone PCM HX for 1000 cases with different fluid inlet conditions and HX designs. We also integrated the models with a vapor compression system to predict the compressor energy consumption and total charging time under various conditions. The results show that overall, the black-box model gave more accurate results than the grey-box model. On average, the mean absolute deviation in the PCM HX fluid outlet temperature was 0.05 K and 0.1 K for the black-box model and grey-box model, respectively. The grey-box model gave larger temperature deviation toward the end of the phase change process, due to the simplified two-node PCM representation. On the system level, the mean absolute deviation in compressor energy consumption was 0.2% and 0.3% for the black-box model and grey-box model, respectively. Their mean absolute deviation in total charging time was 1.1% and 2.6%, respectively. In terms of computation efficiency, the system simulation speedup ratio gained by using the reduced-order models was 11 to 57. System simulation time was decreased from an average of 1465 s to an average of 59 s. This shows that the proposed reduced-order modeling methods can be used to predict system performance of PCM HXs with less than 3% accuracy penalty, and 25 times less computational time than finite-volume models, enabling faster design and evaluation of PCM thermal storage devices.

25 ENERGY STORAGE↗

Dielectric strength of noble and quenched gases for high pressure time projection chambers

Abstract Dielectric breakdown strength is one of the critical performance metrics for pure gases and gas mixtures used in large, high pressure gas time projection chambers. In this paper we experimentally study dielectric breakdown strengths of several important time projection chamber working gases and gas-phase insulators over the pressure range 100 mbar to 10 bar, and gap sizes ranging from 0.1 to 10 mm. Gases characterized include argon, xenon, CO $$_2$$ 2 , CF $$_4$$ 4 , and mixtures 90-10 argon-CH $$_4$$ 4 , 90-10 argon-CO $$_2$$ 2 and 99-1 argon-CF $$_4$$ 4 . We develop a theoretical model for high voltage breakdown based on microphysical simulations that use electron swarm Monte Carlo results as input to Townsend- and Meek-like discharge criteria. This model is shown to be highly predictive at high pressure, out-performing traditional Paschen–Townsend and Meek–Raether models significantly. At lower pressure-times-distance, the Townsend-like model is an excellent description for noble gases whereas the Meek-like model provides a highly accurate prediction for insulating gases.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Development of a rate-based ENRTL-RK process model for a water-lean solvent

Advanced water-lean solvents (WLS) for post-combustion CO2 capture offer several advantages over the aqueous amine solvents . WLS have lower parasitic energy penalty, lower corrosion, lower temperature and high-pressure CO2 regeneration leading to lower cost of CO2 capture. RTI International, with funding from the US Department of Energy, has been developing its novel water-lean solvent, that has shown specific reboiler duty of 2.3 GJ/t-CO2 at the 60-kWe pilot testing unit (Tiller Plant, SINTEF, Norway) and 2.6 GJ/t-CO2 at the engineering scale testing system (12 MWe) at the Technology Centre Mongstad (TCM) in Norway. All heat duties, including the one from TCM testing, were consistent with Aspen Plus modeling of the specific configuration of each test plant. This work focuses on the development of a detailed process model using in-house laboratory measurements and process data at pilot scale. The eNTRL-RK model used in this work is based on an unsymmetric activity coefficient model with the reference states chosen to be pure liquids for solvents and ideal dilute solution at unit solute molality (resulting in activity coefficient of unity at infinite dilution) for electrolytes. It uses the Redlich-Kwong equation of state for vapor phase properties and Henry’s law for solubility of supercritical gases. The model was validated using process data from the pilot-scale campaign at the Tiller plant, and the engineering scale test campaign at TCM. Data on CO2 capture rate, absorber, and regenerator temperature profiles and specific reboiler duties from two different test campaigns at Tiller and TCM, were used to further refine and validate the model and the model compares favorably to experimental data. The validation results against TCM campaign will be presented in this work.

CO2 capture↗

Resilient Operation of Networked Community Microgrids with High Solar Penetration

This project, funded by the US Department of Energy’s Solar Energy Technologies Office (SETO), focused on the operation of microgrids as a coordinated network. The primary objective, which was successfully achieved, was to develop both control strategies and hardware solutions to support the resilient and efficient operation of networked microgrids with high solar penetration. The work was structured around the following four main tasks: • Development of distributed and scalable optimization algorithms for AC-coupled networked microgrids. • Design and implementation of a novel DC interconnection hardware to enable precise power exchange between microgrids. • Laboratory operational validation of the developed technologies using 480 V testbeds and commercially available hardware. • Field operational validation of the complete solution in Adjuntas, Puerto Rico, interconnecting two kW-scale, split-phase microgrids of Casa Pueblo’s microgrids. This project addressed multiple technical challenges across the domains of optimization, control, hardware interconnection, and protection. One of its key contributions was delivering tangible, real-world solutions for networking microgrids. In contrast to purely theoretical or simulation-based work, this project included full-scale hardware operational validation both in the lab and in the field. The work conducted as part of this project—in collaboration with the University of Puerto Rico; the University of Tennessee, Knoxville; the University of Central Florida; and Casa Pueblo—has advanced the state of the art in networked microgrids. Key contributions include the development of distributed control strategies, practical solutions for real-world implementation challenges, and the introduction of a novel DC interlink approach for microgrid interconnection. The project featured both laboratory and field validation using commercial off-the-shelf components. The field deployment successfully validated that a group of microgrids can operate in a coordinated manner, enabling precise power flow between systems and mutual support during extreme events. This project resulted in 15 journal publications and 15 conference papers; 5 graduate students and 15 undergraduate students were supported. The codes of distributed optimization and forecasting were made open-source through OSTI.gov for distributed optimization and forecasting. All the publications are available in the ORNL-hosted project landing page. The DC interlink with state-of-charge balancing control was operationally validated in Adjuntas by interconnecting two real-world, 240 V split-phase microgrids. To the best knowledge of the team, this represents the first operational validation of AC microgrids interconnected via DC-interlinks. As a culmination of this project, a follow-on grant was awarded to support the technology transfer of the distributed optimization framework to a commercial microgrid controller, Stellar Edge, developed by the California-based company New Sun Road.

14 SOLAR ENERGY↗

Surface modification of ZIF ‐90 with triptycene for enhanced interfacial interaction in mixed‐matrix membranes for gas separation

Abstract Zeolite imidazole framework (ZIF‐90) nanoparticles were chemically modified by grafting triptycene moieties. The modified nanoparticles were introduced into a triptycene‐based polyimide as fillers to generate mixed matrix membranes (MMMs) for gas separation. The incorporation of “hook‐like” triptycene moieties in both dispersed and continuous phases led to intimate contact between the two phases and thus defect‐free interfacial morphology, due to the supramolecular interlocking and π–π stacking interaction between triptycene units presented in both phases. The filler/polymer solution showed shear thickening behavior due to such strong interfacial interaction. The separation performance of the prepared composite membranes was investigated as a function of filler loading and particle surface grafting density. Pure‐gas permeation results showed that the gas permeabilities increased expectedly as the filler loading increased, with stable or improved selectivities. The reduced permeability relative to pristine polyimide film is likely due to the pore blockage of ZIF‐90 upon grafting triptycene moieties on the particle surface. Reducing the grafting density of triptycene moieties led to improved permeability and selectivity suggesting good tunability of this series of new composite membranes. Overall, modification of nanofiller with hierarchical triptycene moieties offers a fundamentally new avenue for creation of composite membranes with unique properties in gas separations.

Zhang, Qinnan↗

Element-Specific Study of Magnetic Anisotropy and Hardening in SmCo 5– x Cu x Thin Films

This work investigates the effect of copper substitution on the magnetic properties of SmCo 5 thin films synthesized by molecular beam epitaxy. A series of thin films with varying concentrations of Cu were grown under otherwise identical conditions to disentangle structural and compositional effects on the magnetic behavior. The combined experimental and theoretical studies show that Cu substitution at the Co 3g sites not only stabilizes the formation of the SmCo 5 structure but also enhances magnetic anisotropy and coercivity. Density functional theory calculations indicate that Sm(Co 4 Cu 3g ) 5 possesses a higher single-ion anisotropy as compared to pure SmCo 5 . In addition, X-ray magnetic circular dichroism reveals that Cu substitution causes an increasing decoupling of the Sm 4f and Co 3d moments. Scanning transmission electron microscopy confirms predominantly SmCo 5 phase formation and reveals nanoscale inhomogeneities in the Cu and Co distribution. Our study based on thin film model systems and advanced characterization as well as modeling reveals novel aspects of the complex interplay of intrinsic and extrinsic contributions to magnetic hysteresis in rare-earth-based magnets, i.e., the combination of increased intrinsic anisotropy due to Cu substitution and the extrinsic effect of inhomogeneous elemental distribution of Cu and Co.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Contact Freezing of Water Droplets by Crystalline Organic Acids

The ability of water to freeze into ice crystals in mixed-phase clouds affects physical properties, including particle size, precipitation rates, and radiative properties. The presence of an insoluble particle at the surface of water droplets can promote ice nucleation at temperatures higher than that of pure water, even in the absence of a collision. However, contact freezing remains an underexplored mode of ice nucleation. Here, we present a study of atmospherically relevant organic acids and their role as effective ice-nucleating particles (INP) in contact mode using a Raman-microscope-equipped environmental chamber. We determined contact freezing temperatures induced by solid crystals of docosanol, adipic acid, cis-pinonic acid, fumaric acid, 4-hydroxybenzoic acid, palmitic acid, phthalic acid, sebacic acid, stearic acid, terephthalic acid, and vanillic acid. All solids except fumaric acid promoted contact freezing of water droplets at significantly higher temperatures than pure water in the chamber (−15.0 to −18.5 °C vs −21.3 °C). Physical and chemical properties were identified which correlate with greater effectiveness of INPs in the contact mode, including crystal lattice mismatch with ice, carbon number, and insolubility in water. In conclusion, we suggest that the presence of these organic solids in atmospheric aerosols may promote atmospheric ice nucleation at warm temperatures.

Clouds↗