Rapid freezing of water under dynamic compression

Min S.H., Berkowitz M.L.

We performed molecular dynamics simulations to study how well some of the water models used in simulations describe shocked states. Water in our simulations was described using three different models. One was an often-used all-atom TIP4P/2005 model, while the other two were coarse-grained models used with the MARTINI force field: non-polarizable and polarizable MARTINI water. The all-atom model provided results in good agreement with Hugoniot curves (for data on pressure versus specific volume or, equivalently, on shock wave velocity versus “piston” velocity) describing shocked states in the whole range of pressures (up to 11 GPa) under study. If simulations of shocked states of water using coarse-grained models were performed for short time periods, we observed that data obtained for shocked states at low pressure were fairly accurate compared to experimental Hugoniot curves. Polarizable MARTINI water still provided a good description of Hugoniot curves for pressures up to 11 GPa, while the results for the non-polarizable MARTINI water substantially deviated from the Hugoniot curves. We also calculated the temperature of the Hugoniot states and observed that for TIP4P/2005 water, they were consistent with those from theoretical calculations, while both coarse-grained models predicted much higher temperatures. These high temperatures for MARTINI water can be explained by the loss of degrees of freedom due to coarse-graining procedure.

Tschauner O., Huang S., Greenberg E., Prakapenka V.B., Ma C., Rossman G.R., Shen A.H., Zhang D., Newville M., Lanzirotti A., Tait K.

Encapsulating Earth's deep water filter Small inclusions in diamonds brought up from the mantle provide valuable clues to the mineralogy and chemistry of parts of Earth that we cannot otherwise sample. Tschauner et al. found inclusions of the high-pressure form of water called ice-VII in diamonds sourced from between 410 and 660 km depth, the part of the mantle known as the transition zone. The transition zone is a region where the stable minerals have high water storage capacity. The inclusions suggest that local aqueous pockets form at the transition zone boundary owing to the release of chemically bound water as rock cycles in and out of this region. Science, this issue p. 1136 The presence of ice-VII in diamond inclusions requires regions of the mantle with a free aqueous phase. Water-rich regions in Earth’s deeper mantle are suspected to play a key role in the global water budget and the mobility of heat-generating elements. We show that ice-VII occurs as inclusions in natural diamond and serves as an indicator for such water-rich regions. Ice-VII, the residue of aqueous fluid present during growth of diamond, crystallizes upon ascent of the host diamonds but remains at pressures as high as 24 gigapascals; it is now recognized as a mineral by the International Mineralogical Association. In particular, ice-VII in diamonds points toward fluid-rich locations in the upper transition zone and around the 660-kilometer boundary.

Yang F., Cruikshank O., He W., Kostinski A., Shaw R.A.

Ice nucleation is the crucial step for ice formation in atmospheric clouds and therefore underlies climatologically relevant precipitation and radiative properties. Progress has been made in understanding the roles of temperature, supersaturation, and material properties, but an explanation for the efficient ice nucleation occurring when a particle contacts a supercooled water drop has been elusive for over half a century. Here, we explore ice nucleation initiated at constant temperature and observe that mechanical agitation induces freezing of supercooled water drops at distorted contact lines. Results show that symmetric motion of supercooled water on a vertically oscillating substrate does not freeze, no matter how we agitate it. However, when the moving contact line is distorted with the help of trace amounts of oil or inhomogeneous pinning on the substrate, freezing can occur at temperatures much higher than in a static droplet, equivalent to ∼10^{10} increase in nucleation rate. Several possible mechanisms are proposed to explain the observations. One plausible explanation among them, decreased pressure due to interface curvature, is explored theoretically and compared with the observational results quasiquantitatively. Indeed, the observed freezing-temperature increase scales with contact line speed in a manner consistent with the pressure hypothesis. Whatever the mechanism, the experiments demonstrate a strong preference for ice nucleation at three-phase contact lines compared to the two-phase interface, and they also show that movement and distortion of the contact line are necessary contributions to stimulating the nucleation process.

Millot M., Hamel S., Rygg J.R., Celliers P.M., Collins G.W., Coppari F., Fratanduono D.E., Jeanloz R., Swift D.C., Eggert J.H.

In stark contrast to common ice, Ih, water ice at planetary interior conditions has been predicted to become superionic with fast-diffusing (that is, liquid-like) hydrogen ions moving within a solid lattice of oxygen. Likely to constitute a large fraction of icy giant planets, this extraordinary phase has not been observed in the laboratory. Here, we report laser-driven shock-compression experiments on water ice VII. Using time-resolved optical pyrometry and laser velocimetry measurements as well as supporting density functional theory–molecular dynamics (DFT-MD) simulations, we document the shock equation of state of H2O to unprecedented extreme conditions and unravel thermodynamic signatures showing that ice melts near 5,000 K at 190 GPa. Optical reflectivity and absorption measurements also demonstrate the low electronic conductivity of ice, which, combined with previous measurements of the total electrical conductivity under reverberating shock compression, provides experimental evidence for superionic conduction in water ice at planetary interior conditions, verifying a 30-year-old prediction. Although predicted to occur in planetary interiors, superionic water ice has proved elusive to identify experimentally. Laser-driven shock-compression experiments on water ice VII now verify its existence.

Rao F., Ding K., Zhou Y., Zheng Y., Xia M., Lv S., Song Z., Feng S., Ronneberger I., Mazzarello R., Zhang W., Ma E.

Fast phase change with no preconditions Random access memory (RAM) devices that rely on phase changes are primarily limited by the speed of crystallization. Rao et al. combined theory with a simple set of selection criteria to isolate a scandium-doped antimony telluride (SST) with a subnanosecond crystallization speed (see the Perspective by Akola and Jones). They synthesized SST and constructed a RAM device with a 700-picosecond writing speed. This is an order of magnitude faster than previous phase-change memory devices and competitive with consumer dynamic access, static random access, and flash memory. Science, this issue p. 1423; see also p. 1386 Computer-aided materials design helps to identify a subnanosecond phase-change random-access memory material. Operation speed is a key challenge in phase-change random-access memory (PCRAM) technology, especially for achieving subnanosecond high-speed cache memory. Commercialized PCRAM products are limited by the tens of nanoseconds writing speed, originating from the stochastic crystal nucleation during the crystallization of amorphous germanium antimony telluride (Ge2Sb2Te5). Here, we demonstrate an alloying strategy to speed up the crystallization kinetics. The scandium antimony telluride (Sc0.2Sb2Te3) compound that we designed allows a writing speed of only 700 picoseconds without preprogramming in a large conventional PCRAM device. This ultrafast crystallization stems from the reduced stochasticity of nucleation through geometrically matched and robust scandium telluride (ScTe) chemical bonds that stabilize crystal precursors in the amorphous state. Controlling nucleation through alloy design paves the way for the development of cache-type PCRAM technology to boost the working efficiency of computing systems.

Zepeda-Ruiz L.A., Sadigh B., Chernov A.A., Haxhimali T., Samanta A., Oppelstrup T., Hamel S., Benedict L.X., Belof J.L.

Molecular dynamics simulations of an embedded atom copper system in the isobaric-isenthalpic ensemble are used to study the effective solid-liquid interfacial free energy of quasi-spherical solid crystals within a liquid. This is within the larger context of molecular dynamics simulations of this system undergoing solidification, where single individually prepared crystallites of different sizes grow until they reach a thermodynamically stable final state. The resulting equilibrium shapes possess the full structural details expected for solids with weakly anisotropic surface free energies (in these cases, ∼5% radial flattening and rounded [111] octahedral faces). The simplifying assumption of sphericity and perfect isotropy leads to an effective interfacial free energy as appearing in the Gibbs-Thomson equation, which we determine to be ∼177 erg/cm2, roughly independent of crystal size for radii in the 50–250 Å range. This quantity may be used in atomistically informed models of solidification kinetics for this system.

Lupi L., Hudait A., Peters B., Grünwald M., Gotchy Mullen R., Nguyen A.H., Molinero V.

Stacking-disordered ice crystallites are shown to have an ice nucleation rate much higher than predicted by classical nucleation theory, which needs to be taken into account in cloud modelling. Water freezing is crucial to Earth's climate, and accurate weather and climate forecasts depend on reliable predictions of ice nucleation rates. Such predictions are typically based on classical nucleation theory, which assumes that the structure of the initially formed ice crystallites corresponds to that of thermodynamically stable hexagonal ice. Laura Lupi et al. now report simulations and energy calculations with a simple water model to show that, for emerging crystallites, ice with disordered stacking is more stable than hexagonal ice and results in ice nucleation rates more than three orders of magnitude higher than predicted by classical nucleation theory. This effect must be accounted for in cloud models and when interpreting ice nucleation rates measured in laboratory conditions and extrapolating them to temperatures important to clouds. The freezing of water affects the processes that determine Earth’s climate. Therefore, accurate weather and climate forecasts hinge on good predictions of ice nucleation rates1. Such rate predictions are based on extrapolations using classical nucleation theory1,2, which assumes that the structure of nanometre-sized ice crystallites corresponds to that of hexagonal ice, the thermodynamically stable form of bulk ice. However, simulations with various water models find that ice nucleated and grown under atmospheric temperatures is at all sizes stacking-disordered, consisting of random sequences of cubic and hexagonal ice layers3,4,5,6,7,8. This implies that stacking-disordered ice crystallites either are more stable than hexagonal ice crystallites or form because of non-equilibrium dynamical effects. Both scenarios challenge central tenets of classical nucleation theory. Here we use rare-event sampling9,10,11 and free energy calculations12 with the mW water model13 to show that the entropy of mixing cubic and hexagonal layers makes stacking-disordered ice the stable phase for crystallites up to a size of at least 100,000 molecules. We find that stacking-disordered critical crystallites at 230 kelvin are about 14 kilojoules per mole of crystallite more stable than hexagonal crystallites, making their ice nucleation rates more than three orders of magnitude higher than predicted by classical nucleation theory. This effect on nucleation rates is temperature dependent, being the most pronounced at the warmest conditions, and should affect the modelling of cloud formation and ice particle numbers, which are very sensitive to the temperature dependence of ice nucleation rates1. We conclude that classical nucleation theory needs to be corrected to include the dependence of the crystallization driving force on the size of the ice crystallite when interpreting and extrapolating ice nucleation rates from experimental laboratory conditions to the temperatures that occur in clouds.

Hazael R., Fitzmaurice B.C., Foglia F., Appleby-Thomas G.J., McMillan P.F.

The possibility that life can exist within previously unconsidered habitats is causing us to expand our understanding of potential planetary biospheres. Significant populations of living organisms have been identified at depths extending up to several km below the Earth's surface; whereas laboratory experiments have shown that microbial species can survive following exposure to GigaPascal (GPa) pressures. Understanding the degree to which simple organisms such as microbes survive such extreme pressurization under static compression conditions is being actively investigated. The survival of bacteria under dynamic shock compression is also of interest. Such studies are being partly driven to test the hypothesis of potential transport of biological organisms between planetary systems. Shock compression is also of interest for the potential modification and sterilization of foodstuffs and agricultural products. Here we report the survival of Shewanella oneidensis bacteria exposed to dynamic (shock) compression. The samples examined included: (a) a “wild type” (WT) strain and (b) a “pressure adapted” (PA) population obtained by culturing survivors from static compression experiments to 750 MPa. Following exposure to peak shock pressures of 1.5 and 2.5 GPa the proportion of survivors was established as the number of colony forming units (CFU) present after recovery to ambient conditions. The data were compared with previous results in which the same bacterial samples were exposed to static pressurization to the same pressures, for 15 minutes each. The results indicate that shock compression leads to survival of a significantly greater proportion of both WT and PA organisms. The significantly shorter duration of the pressure pulse during the shock experiments (2–3 µs) likely contributes to the increased survival of the microbial species. One reason for this can involve the crossover from deformable to rigid solid-like mechanical relaxational behavior that occurs for bacterial cell walls on the order of seconds in the time-dependent strain rate.

Myint P.C., Benedict L.X., Belof J.L.

We present equations of state relevant to conditions encountered in ramp and multiple-shock compression experiments of water. These experiments compress water from ambient conditions to pressures as high as about 14 GPa and temperatures of up to several hundreds of Kelvin. Water may freeze into ice VII during this process. Although there are several studies on the thermodynamic properties of ice VII, an accurate and analytic free energy model from which all other properties may be derived in a thermodynamically consistent manner has not been previously determined. We have developed such a free energy model for ice VII that is calibrated with pressure-volume-temperature measurements and melt curve data. Furthermore, we show that liquid water in the pressure and temperature range of interest is well-represented by a simple Mie-Grüneisen equation of state. Our liquid water and ice VII equations of state are validated by comparing to sound speed and Hugoniot data. Although they are targeted towards ramp and multiple-shock compression experiments, we demonstrate that our equations of state also behave reasonably well at pressures and temperatures that lie somewhat beyond those found in the experiments.

Hirata M., Yagasaki T., Matsumoto M., Tanaka H.

We report a new ice phase that forms spontaneously at the interface between ice VII and liquid water in molecular dynamics simulations of TIP4P/2005 water. The new phase is structurally quite similar to an ice phase originally found to be a precursor in the course of the homogeneous nucleation of ice VII in liquid water. A part of the water molecules in these ice phases can rotate easily because the number of hydrogen bonds in them is less than four, and thus they can be regarded as partial plastic phases. A rough estimate suggests that these phases are thermodynamically more stable than either ice VI or ice VII for 3 GPa < P < 18 GPa at T = 300 K. Although the partial plastic phases would be metastable states at any point in the phase diagram of real water, they might be realized experimentally with the aid of dopants and/or solid surfaces.

Gleason A. ., Bolme C. ., Galtier E., Lee H. ., Granados E., Dolan D. ., Seagle C. ., Ao T., Ali S., Lazicki A., Swift D., Celliers P., Mao W. .

Time-resolved x-ray diffraction (XRD) of compressed liquid water shows transformation to ice VII in 6 nsec, revealing crystallization rather than amorphous solidification during compression freezing. Application of classical nucleation theory indicates heterogeneous nucleation and one-dimensional (e.g., needlelike) growth. These first XRD data demonstrate rapid growth kinetics of ice VII with implications for fundamental physics of diffusion-mediated crystallization and thermodynamic modeling of collision or impact events on ice-rich planetary bodies.

Bi Y., Cao B., Li T.

The freezing of water typically proceeds through impurity-mediated heterogeneous nucleation. Although non-planar geometry generically exists on the surfaces of ice nucleation centres, its role in nucleation remains poorly understood. Here we show that an atomically sharp, concave wedge can further promote ice nucleation with special wedge geometries. Our molecular analysis shows that significant enhancements of ice nucleation can emerge both when the geometry of a wedge matches the ice lattice and when such lattice match does not exist. In particular, a 45° wedge is found to greatly enhance ice nucleation by facilitating the formation of special topological defects that consequently catalyse the growth of regular ice. Our study not only highlights the active role of defects in nucleation but also suggests that the traditional concept of lattice match between a nucleation centre and crystalline lattice should be extended to include a broader match with metastable, non-crystalline structural motifs. Understanding ice nucleation is important for the development of accurate cloud models. Here Biet al. show that sharp wedges can enhance ice nucleation both when the wedge geometry matches the ice lattice and when such matching is absent, in which case nucleation is promoted by topological defects.

Pham C.H., Reddy S.K., Chen K., Knight C., Paesani F.

Many-body effects in ice are investigated through a systematic analysis of the lattice energies of several proton ordered and disordered phases, which are calculated with different flexible water models, ranging from pairwise additive (q-TIP4P/F) to polarizable (TTM3-F and AMOEBA) and explicit many-body (MB-pol) potential energy functions. Comparisons with available experimental and diffusion Monte Carlo data emphasize the importance of an accurate description of the individual terms of the many-body expansion of the interaction energy between water molecules for the correct prediction of the energy ordering of the ice phases. Further analysis of the MB-pol results, in terms of fundamental energy contributions, demonstrates that the differences in lattice energies between different ice phases are sensitively dependent on the subtle balance between short-range two-body and three-body interactions, many-body induction, and dispersion energy. By correctly reproducing many-body effects at both short range and long range, it is found that MB-pol accurately predicts the energetics of different ice phases, which provides further support for the accuracy of MB-pol in representing the properties of water from the gas to the condensed phase.

Haxhimali T., Belof J.L., Benedict L.X.

Phase-field models have become popular in the last two decades to describe a host of free-boundary problems. The strength of the method relies on implicitly describing the dynamics of surfaces and interfaces by a continuous scalar field that enters the global grand free energy functional of the system. Here we explore the potential utility of this method in order to describe shock-induced phase transitions. To this end we make use of the Multiphase Field Theory (MFT) to account for the existence of multiple phases during the transition, and we couple MFT to a hydrodynamic model in the context of a new LLNL code for phase transitions, SAMSA. As a demonstration of this approach, we apply our code to the α − ε-Fe phase transition under shock wave loading conditions and compare our results with experiments of Jensen et. al. [J. Appl. Phys., 105:103502 (2009)] and Barker and Hollenbach [J. Appl. Phys., 45:4872 (1974)].

Stafford S.J., Chapman D.J., Bland S.N., Eakins D.E.

Water can freeze upon multiple shock compression, but the window material determines the pressure of the phase transition. Several plate impact experiments were conducted with liquid targets on a single-stage gas gun, diagnosed simultaneously using photonic doppler velocimetry (PDV) and high speed imaging through the water. The experiments investigated why silica windows instigate freezing above 2.5 GPa whilst sapphire windows do not until 7 GPa. We find that the nucleation of ice occurs on the surfaces of windows and can be affected by the surface coating suggesting the surface energy of fused silica, likely due to hydroxyl groups, encourages nucleation of ice VII crystallites. Aluminium coatings prevent nucleation and sapphire surfaces do not nucleate until approximately 6.5 GPa. This is believed to be the threshold pressure for the homogeneous nucleation of water.

Smirnov A., Anisimkin V., Ageykin N., Datsuk E., Kuznetsova I.

An important technical task is to develop methods for recording the phase transitions of water to ice. At present, many sensors based on various types of acoustic waves are suggested for solving this challenge. This paper focuses on the theoretical and experimental study of the effect of water-to-ice phase transition on the properties of Lamb and quasi shear horizontal (QSH) acoustic waves of a higher order propagating in different directions in piezoelectric plates with strong anisotropy. Y-cut LiNbO3, 128Y-cut LiNbO3, and 36Y-cut LiTaO3 plates with a thickness of 500 μm and 350 μm were used as piezoelectric substrates. It was shown that the amplitude of the waves under study can decrease, increase, or remain relatively stable due to the water-to-ice phase transition, depending on the propagation direction and mode order. The greatest decrease in amplitude (42.1 dB) due to glaciation occurred for Lamb waves with a frequency of 40.53 MHz and propagating in the YX+30° LiNbO3 plate. The smallest change in the amplitude (0.9 dB) due to glaciation was observed for QSH waves at 56.5 MHz propagating in the YX+60° LiNbO3 plate. Additionally, it was also found that, in the YX+30° LiNbO3 plate, the water-to-ice transition results in the complete absorption of all acoustic waves within the specified frequency range (10–60 MHz), with the exception of one. The phase velocities, electromechanical coupling coefficients, elastic polarizations, and attenuation of the waves under study were calculated. The structures “air–piezoelectric plate–air”, “air–piezoelectric plate–liquid”, and “air–piezoelectric plate–ice” were considered. The results obtained can be used to develop methods for detecting ice formation and measuring its parameters.

Zhang X., Mochizuki K.

We use molecular dynamics simulations to examine the homogeneous nucleation of ice VII from metastable liquid water. An unsupervised machine learning classification identifies two distinct local structures composing Ice VII nuclei. The seeding method, combined with the classical nucleation theory (CNT), predicts the solid–liquid interfacial free energy, consistent with the value from the mold integration method. Meanwhile, the nucleation rates estimated from the CNT framework and brute force spontaneous nucleations are inconsistent, and we discuss the reasons for this discrepancy. Structural and dynamical heterogeneities suggest that the potential birthplace for an ice VII embryo is relatively ordered, although not necessarily relatively immobile. Moreover, we demonstrate that without the formation of hydrogen-bond links, ice VII embryos do not grow.

Wang L., Meng H., Wang F., Liu H.

The freezing of supercooled liquids is closely related to many fields. Vibration is one of the most common mechanical disturbances to induce nucleation. However, there has been no systematic study and understanding of ice nucleation mechanisms and how to maintain the stability of supercooled water under vibration. We studied ice nucleation from water in vials by using mechanical vibration as excitation. The results showed that it accelerates nucleation generally. Nevertheless, as the supercooling or the vibration intensity is low, or the flow is hindered, vibration has little effect on the supercooling stability. More meaningfully, if the flow is completely limited under isochoric conditions, vibration has no effect on the freezing temperature of supercooled water, and ice nucleation depends entirely on the container itself. It was demonstrated that stretching water and the formation of cavitation bubbles are the main factors affecting nucleation. The study further revealed three kinds of ice nucleation mechanisms: wall-contact, negative-pressure, and high-pressure nucleation. The findings are helpful for recognizing the effects of vibration on supercooling related to biological tissue preservation and transportation, energy storage, etc., and contribute to understanding the fundamental nucleation mechanism of the solid phase in supercooled liquids under mechanical disturbances.

Myint P.C., Sterbentz D.M., Brown J.L., Stoltzfus B.S., Delplanque J.R., Belof J.L.

Quasi-isentropic compression enables one to study the solidification of metastable liquid states that are inaccessible through other experimental means. The onset of this nonequilibrium solidification is known to depend on the compression rate and material-specific factors, but this complex interdependence has not been well characterized. In this study, we use a combination of experiments, theory, and computational simulations to derive a general scaling law that quantifies this dependence. One of its applications is a novel means to elucidate melt temperatures at high pressures.

Belof J.L., Murialdo M., Sadigh B.

Insights from non-equilibrium statistical mechanics, highlighting the role of work and fluctuations at the microscale, are applied toward the development of a fundamental, rigorous and purely atomistic theory of nucleation. Nanoscale fluctuations in order, density and heat influence the local nucleation rate by orders of magnitude, necessitating their inclusion through a modern approach. Coarse-graining over the underlying Hamiltonian dynamics allows derivation of a microscale expression for the nucleation rate in terms of a classical path integral over far from equilibrium trajectories and their associated work. Second law violating states at the microscale, as found from the dynamics of small critical nucleation clusters, contribute exponentially to the observable macroscale nucleation rate.

Consiglio A.N., Lilley D., Prasher R., Rubinsky B., Powell-Palm M.J.

Stable aqueous supercooling has shown significant potential as a technique for human tissue preservation, food cold storage, conservation biology, and beyond, but its stochastic nature has made its translation outside the laboratory difficult. In this work, we present an isochoric nucleation detection (INDe) platform for automated, high-throughput characterization of aqueous supercooling at >1 mL volumes, which enables statistically-powerful determination of the temperatures and time periods for which supercooling in a given aqueous system will remain stable. We employ the INDe to investigate the effects of thermodynamic, surface, and chemical parameters on aqueous supercooling, and demonstrate that various simple system modifications can significantly enhance supercooling stability, including isochoric (constant-volume) confinement, hydrophobic container walls, and the addition of even mild concentrations of solute. Finally, in order to enable informed design of stable supercooled biopreservation protocols, we apply a statistical model to estimate stable supercooling durations as a function of temperature and solution chemistry, producing proof-of-concept supercooling stability maps for four common cryoprotective solutes.

Marshall M. ., Millot M., Fratanduono D. ., Sterbentz D. ., Myint P. ., Belof J. ., Kim Y.-., Coppari F., Ali S. ., Eggert J. ., Smith R. ., McNaney J. .

The ubiquitous nature and unusual properties of water have motivated many studies on its metastability under temperature- or pressure-induced phase transformations. Here, nanosecond compression by a high-power laser is used to create the nonequilibrium conditions where liquid water persists well into the stable region of ice VII. Through our experiments, as well as a complementary theoretical-computational analysis based on classical nucleation theory, we report that the metastability limit of liquid water under nearly isentropic compression from ambient conditions is at least 8 GPa, higher than the 7 GPa previously reported for lower loading rates.

Wu L., Ren Y., Liao W., Huang X., Liu F., Zhang M., Sun Y.

The phase transition behaviors of the shocked water are investigated by employing an optical transmittance in-situ detection system. Based on the light scattering theory and phase transformation kinetics, the phase transition mechanism of the water under multiple shocks is discussed. The experimental data indicate that the evolution of the transmittance of the shocked water can be broadly divided into three stages: relaxation stage, decline stage, and recovery stage. In the early stage of the phase transition, the new phase particles began to form around the quartz/window interface. It should be mentioned that the water/ice phase boundary seems to move toward the liquid region in one experiment of this work. Due to the new phase core being much smaller than the wavelength of the incident light, the transmittance of the sample within the relaxation stage remains steady. The decline stage can be divided into the rapid descent stage and the slow descent stage in this work, which is considered as the different growth rates of the new phase particle under different shock loadings. The recovery stage is attributed to the emergence of the new phase particles which are bigger than the critical value. However, the influence of the size growth and the population growth of the new phase particles on the transmittance restrict each other, which may be responsible for the phenomenon that the transmittance curve does not return to the initial level.

Sadigh B., Zepeda-Ruiz L., Belof J.L.

Significance Kinetic stabilization of metastable phases in rapidly cooled metals and alloys has been established in experiments for decades. However, atomistic theories that can quantitatively predict the solidification conditions that produce nonequilibrium phases are still in their infancy. Recent advances in pulsed power/laser technologies, as well as in situ characterization, have brought to bear unprecedented understanding of matter at extreme temperatures and pressures. However, accurate predictions of kinetic stabilization of metastable phases that are necessary for physical interpretation of these experiments are lacking. This work provides a blueprint for development of kinetic phase maps of materials undergoing rapid solidification from first principles. Through atomistic simulations, the phases dominating nucleation are identified, and their kinetic stabilities during the growth stage are characterized.

Anisimkin V., Kolesov V., Kuznetsova A., Shamsutdinova E., Kuznetsova I.

It is shown that, in spite of the wave radiation into the adjacent liquid, a large group of Lamb waves are able to propagate along piezoelectric plates (quartz, LiNbO3, LiTaO3) coated with a liquid layer (distilled water H2O). When the layer freezes, most of the group’s waves increase their losses, essentially forming an acoustic response towards water-to-ice transformation. Partial contributions to the responses originating from wave propagation, electro-mechanical transduction, and wave scattering were estimated and compared with the coupling constants, and the vertical displacements of the waves were calculated numerically at the water–plate and ice–plate interfaces. The maximum values of the responses (20–30 dB at 10–100 MHz) are attributed to the total water-to-ice transformation. Time variations in the responses at intermediate temperatures were interpreted in terms of a two-phase system containing both water and ice simultaneously. The results of the paper may turn out to be useful for some applications where the control of ice formation is an important problem (aircraft wings, ship bodies, car roads, etc.).

Myint P.C., Sadigh B., Benedict L.X., Sterbentz D.M., Hall B.M., Belof J.L.

In this study, we report a numerical scheme to integrate models for the kinetics of solidification processes together with phase-behavior computations in the context of continuum-scale hydrodynamic simulations. The objective of the phase-behavior computations is to determine the pressure and temperature, given the following three sets of inputs: (1) an appropriate equation of state to describe our system, (2) the phase fraction(s) produced by the kinetic models, (3) and the volume and internal energy obtained by solving the conservation equations that govern the hydrodynamic behavior. The kinetics are assumed to be governed by the Kolmogorov–Johnson–Mehl–Avrami equation, and the nucleation and growth rates that enter into that equation are functions of the pressure and temperature produced by the phase-behavior computations. Our formulation allows for the fluid and solid phases to be at different temperatures (thermal nonequilibrium) and pressures (arising from surface-tension-induced Laplace contributions). The formulation is presented in a fairly general setting that is independent of any particular material, although we demonstrate it in some examples related to high-energy-density science applications where materials are rapidly compressed to pressures exceeding several gigapascals in less than a microsecond. We conclude with a critical evaluation of our approach and provide suggestions for future work to improve the predictive capabilities and generality of the models.

Sterbentz D.M., Gambino J.R., Myint P.C., Delplanque J., Springer H.K., Marshall M.C., Belof J.L.

Ramp-wave dynamic-compression experiments are used to examine quasi-isentropic loading paths in materials. The gradual and continuous increase in pressure created by ramp waves make these types of experiments ideal for studying nonequilibrium material behavior, such as solidification kinetics. In ramp-wave compression experiments, the input drive pressure to the experimental setup may be exerted through one of a number of different mechanisms (e.g., magnetic fields, gas-gun-driven impactors, or high-energy lasers) and is generally required for simulating such experiments. Yet, regardless of the specific mechanism, this drive pressure cannot be measured directly (measurements are generally taken at a location near the back of the experimental setup through a transparent window), leading to an inverse problem where one must determine the drive pressure at the front of the experimental setup (i.e., the input) that corresponds to the particle velocity (the output) measured near the back of the experimental setup. We solve this inverse problem using a heuristic optimization algorithm, known as differential evolution, coupled with a multiphysics, hydrodynamics code that simulates the compression of the experimental setup. By running many rounds of forward simulations of the experimental setup, our optimization process iteratively searches for a drive pressure that is optimized to closely reproduce the experimentally measured particle velocity near the back of the experimental setup. While our optimization methodology requires a significant number of hydrodynamics simulations to be conducted, many of these can be performed in parallel, which greatly reduces the time cost of our methodology. One novel aspect of our method for determining the drive pressure is that it does not require physical modeling of the drive mechanism and can thus be broadly applied to many types of ramp-compression experiments, regardless of the drive mechanism.

Consiglio A., Ukpai G., Rubinsky B., Powell-Palm M.J.

This work explores the effects of constant volume confinement on cavitation-induced ice nucleation by marrying fluid dynamics, thermodynamics, and nucleation kinetics into a single approach. The authors find that confinement at even macroscopic volumes can suppress cavitation-induced nucleation from single microscale bubbles, suggesting that macroscale confinement may provide an effective method of suppressing this nucleation pathway in supercooled aqueous systems.

Radousky H.B., Armstrong M.R., Austin R.A., Stavrou E., Brown S., Chernov A.A., Gleason A.E., Granados E., Grivickas P., Holtgrewe N., Lee H.J., Lobanov S.S., Nagler B., Nam I., Prakapenka V., et. al.

This paper studies zirconium subjected to high pressure conditions. Using x-ray diffraction, the authors observe the onset of melting at short times after shocking, and refreeze shortly thereafter. The latent heat of crystallization is found to provide the energy for the recrystallization process

Nissen E.J., Dolan D.H.

Quasi-isentropic compression of liquid water beyond 5 GPa rapidly creates ice VII on 1–10 ns time scales. The onset of this phase transition can be modified by changing the initial temperature of the liquid sample and/or the compression rate. These effects were studied using the Sandia Thor-64 pulsed power machine. Increasing the initial temperature pushes freezing above the previously reported 7 GPa metastable limit. Slower compression allows freezing to occur below the metastable limit, though the compression rate has a greater effect at an elevated temperature than at room temperature.Quasi-isentropic compression of liquid water beyond 5 GPa rapidly creates ice VII on 1–10 ns time scales. The onset of this phase transition can be modified by changing the initial temperature of the liquid sample and/or the compression rate. These effects were studied using the Sandia Thor-64 pulsed power machine. Increasing the initial temperature pushes freezing above the previously reported 7 GPa metastable limit. Slower compression allows freezing to occur below the metastable limit, though the compression rate has a greater effect at an elevated temperature than at room temperature.