SEARCH · Search NASA

Results for “Classical nucleation theory”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

SourceResearch connectionFrom yearThrough year

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 55 records · Page 3

All sources NASA NTRS DOE OSTI

NASA NTRS2015

Thermodynamic Derivation of the Activation Energy for Ice Nucleation

Cirrus clouds play a key role in the radiative and hydrological balance of the upper troposphere. Their correct representation in atmospheric models requires an understanding of the microscopic processes leading to ice nucleation. A key parameter in the theoretical description of ice nucleation is the activation energy, which controls the flux of water molecules from the bulk of the liquid to the solid during the early stages of ice formation. In most studies it is estimated by direct association with the bulk properties of water, typically viscosity and self-diffusivity. As the environment in the ice-liquid interface may differ from that of the bulk, this approach may introduce bias in calculated nucleation rates. In this work a theoretical model is proposed to describe the transfer of water molecules across the ice-liquid interface. Within this framework the activation energy naturally emerges from the combination of the energy required to break hydrogen bonds in the liquid, i.e., the bulk diffusion process, and the work dissipated from the molecular rearrangement of water molecules within the ice-liquid interface. The new expression is introduced into a generalized form of classical nucleation theory. Even though no nucleation rate measurements are used to fit any of the parameters of the theory the predicted nucleation rate is in good agreement with experimental results, even at temperature as low as 190 K, where it tends to be underestimated by most models. It is shown that the activation energy has a strong dependency on temperature and a weak dependency on water activity. Such dependencies are masked by thermodynamic effects at temperatures typical of homogeneous freezing of cloud droplets; however, they may affect the formation of ice in haze aerosol particles. The new model provides an independent estimation of the activation energy and the homogeneous ice nucleation rate, and it may help to improve the interpretation of experimental results and the development of parameterizations for cloud formation.

Cirrus clouds↗

NASA NTRS2020

Ultrafast Melting at Metal-Semiconductor Interfaces: A Molecular Dynamics Study

Quantifying the thermodynamics of interfacial melting is important for several applications such as laser machining and designing radiation hardened electronic devices. Due to the short time and length scales that are involved in the process, molecular simulations provide an ideal path for understating the interfacial melting phenomena. In this work we investigate tungsten (W) – silicon carbide (SiC) interfaces which are relevant in modern high-power electronic devices. Classical molecular dynamics simulations along with the two-temperature model (TTM) were used to study the radiation induced melting of the interface while a neural network-based machine learning framework was used to track the transient re-crystallization process. The damage endured by the semiconductor at the interface following the radiation event is discussed in detail while the re-crystallization of the metal is described in terms of the classical nucleation theory.

Ashwin Ravichandran↗

NASA NTRSDate not supplied

Inefficient Growth of Refractory Grains: Implications for Grains in the Solar Nebula

Introduction: We report the results of a sounding rocket experiment in which SiO nucleation and growth in an argon atmosphere was observed in microgravity starting from a vapor generated by evaporation of waterglass deposited on a heated Ta wire. The temperature and pressure at the point of nucleation was determined using a double wavelength Mach–Zehnder-type interferometer. The particle composition and grain size distribution were measured after payload recovery using a Transmission Electron Microscope (TEM; JEM-2100F. JEOL Ltd., Tokyo). The results were analyzed using Modified Classical Nucleation Theory (MCNT)[1]. We report a measurement of the SiO-silicate grain sticking coefficient of 0.016, indicating very inefficient grain growth from the vapor. In other words, for every 100 SiO molecules that collide with a growing grain only one to two are captured. In the only two previous studies of the growth of solid particles from the gas phase the calculated sticking coefficients were much lower. For zinc atoms colliding with zinc crystals only three out of 100,000 collisions resulted in grain growth [2]. Iron atoms colliding with growing iron particles similarly showed an efficiency of ~0.00002 [3]. For zinc, we can explain inefficient growth due to the difficulty of the colliding atom coming upon a vacancy in the growing crystal lattice before it evaporates from the grain surface. The much higher sticking coefficient of SiO molecules on silica grains is reasonable because the silica grains are highly amorphous or glassy and therefore provide a much higher defect density where SiO molecules can be captured into the grains. In the case of similar Fe experiment, the critical cluster was the dimer. In this case the forming dimer returns to the vapor phase by dissociation due to the excess energy from the formation of the Fe-Fe bond.

Joseph A Nuth↗

NASA NTRS2022

The impacts of immersion ice nucleation parameterizations on Arctic mixed-phase stratiform cloud properties and the Arctic radiation budget in GEOS-5

The influence of four different immersion freezing parameterizations on Arctic clouds and the top-of-the atmosphere (TOA) and surface radiation fluxes is investigated in the fifth version of the National Aeronautics and Space Administration (NASA) Goddard Earth Observing System (GEOS-5) with sea surface temperature, sea ice fraction and aerosol emissions held fixed. The different parameterizations were derived from a variety of sources, including classical nucleation theory, field and laboratory measurements. Despite the large spread in the ice-nucleating particle (INP) concentrations in the parameterizations, the cloud properties and radiative fluxes had a tendency to form two groups, with the lower INP concentration category producing larger water path and low-level cloud fraction during winter and early spring, whereas the opposite occurred during the summer season. The stability of the lower troposphere was found to strongly correlate with low-cloud fraction, and along with the effect of ice nucleation, ice sedimentation and melting rates, appears to explain the spring-to-summer reversal pattern in the relative magnitude of the cloud properties between the two categories of simulations. The strong modulation effect of the liquid phase on immersion freezing led to the successful simulation of the characteristic Arctic cloud structure, with a layer rich in supercooled water near cloud top and ice and snow at lower levels. Comparison with satellite retrievals and in situ data suggest that simulations with low INP concentrations more realistically represent Arctic clouds and radiation.

Arctic↗

NASA NTRS2023

A 1D Model for Nucleation of Ice From Aerosol Particles: An Application to a Mixed-Phase Arctic Stratus Cloud Layer

Mixed-phase clouds (MPCs) have been identified as significant contributors to uncertainties in climate projections, attributable to model representation of processes controlling the formation and loss of supercooled water droplets and ice particles from the atmosphere. Arctic MPCs are commonly widespread and long-lived, with sustained ice crystal formation processes that challenge current understanding. This study examines the ice-nucleating particle (INP) reservoir dynamics governing immersion-mode heterogeneous freezing in an observed case of Arctic MPCs using a simplified 1D aerosol-cloud model. The model setup includes prescribed dynamical forcings and thermodynamic profiles, and represents INPs as multicomponent and polydisperse particle size distributions. Diagnostic and prognostic approaches to immersion freezing parameterization are compared, including time-independent (singular) number- and surface area-based descriptions and a time-dependent description following classical nucleation theory (CNT). The choice of freezing parameterization defines the size of the INP reservoir. The CNT-based description yields an orders of magnitude larger INP reservoir than the singular parameterizations, which is the dominant factor for sustained ice crystal formation. The efficiency of the freezing process and cloud cooling are of secondary importance. A diagnostic treatment neglecting INP loss is only accurate when the INP reservoir size is large and INP depletion weak. Since a larger INP reservoir sustains ice crystal formation substantially longer, and ice water path scales with ice crystal concentrations for the conditions considered, resolving the source of differences in INP reservoir dynamics due to model implementation is a high priority for advancing climate model physics.

aerosol↗

NASA NTRS1992

Estimation of the nucleation rate by differential scanning calorimetry

A realistic computer model is presented for calculating the time-dependent volume fraction transformed during the devitrification of glasses, assuming the classical theory of nucleation and continuous growth. Time- and cluster-dependent nucleation rates are calculated by modeling directly the evolving cluster distribution. Statistical overlap in the volume fraction transformed is taken into account using the standard Johnson-Mehl-Avrami formalism. Devitrification behavior under isothermal and nonisothermal conditions is described. The model is used to demonstrate that the recent suggestion by Ray and Day (1990) that nonisothermal DSC studies can be used to determine the temperature for the peak nucleation rate, is qualitatively correct for lithium disilicate, the glass investigated.

Kelton, Kenneth F.↗

NASA NTRS1991

Homogeneous freezing nucleation of stratospheric solution droplets

The classical theory of homogeneous nucleation was used to calculate the freezing rate of sulfuric acid solution aerosols under stratospheric conditions. The freezing of stratospheric aerosols would be important for the nucleation of nitric acid trihydrate particles in the Arctic and Antarctic stratospheres. In addition, the rate of heterogeneous chemical reactions on stratospheric aerosols may be very sensitive to their state. The calculations indicate that homogeneous freezing nucleation of pure water ice in the stratospheric solution droplets would occur at temperatures below about 192 K. However, the physical properties of H2SO4 solution at such low temperatures are not well known, and it is possible that sulfuric acid aerosols will freeze out at temperatures ranging from about 180 to 195 K. It is also shown that the temperature at which the aerosols freeze is nearly independent of their size.

Jensen, Eric J.↗

NASA NTRS1996

First Measurements of Time-Dependent Nucleation as a Function of Composition in Na2O.2CaO.3SiO2 Glasses

The first measurements in any system of the composition dependence of the time-dependent nucleation rate are presented Nucleation rates of the stoichiometric crystalline phase, Na2O.2CaO.3SiO2, from quenched glasses made with different SiO2 concentrations were determined as a function of temperature and glass composition. A strong compositional dependence of the nucleation rates and a weak dependence for the induction times are observed. Using measured values of the liquidus temperatures and growth velocities as a function of glass composition, these data are shown to be consistent with predictions from the classical theory of nucleation, assuming a composition-dependent interfacial energy.

Kelton, K. F.↗

NASA NTRS2003

Kinetics of Nucleation and Crystal Growth in Glass Forming Melts in Microgravity

This flight definition project has the specific objective of investigating the kinetics of nucleation and crystal growth in high temperature inorganic oxide, glass forming melts in microgravity. It is related to one1 of our previous NASA projects that was concerned with glass formation for high temperature containerless melts in microgravity. The previous work culminated in two experiments which were conducted aboard the space shuttle in 1983 and 1985 and which consisted of melting (at 1500 C) and cooling levitated 6 to 8 mm diameter spherical samples in a Single Axis Acoustic Levitator (SAAL) furnace. Compared to other types of materials, there have been relatively few experiments, 6 to 8, conducted on inorganic glasses in space. These experiments have been concerned with mass transport (alkali diffusion), containerless melting, critical cooling rate for glass formation, chemical homogeneity, fiber pulling, and crystallization of glass forming melts. One of the most important and consistent findings in all of these experiments has been that the glasses prepared in microgravity are more resistant to crystallization (better glass former) and more chemically homogeneous than equivalent glasses made on earth (1g). The chemical composition of the melt appears relatively unimportant since the same general results have been reported for oxide, fluoride and chalcogenide melts. These results for space-processed glasses have important implications, since glasses with a higher resistance to crystallization or higher chemical homogeneity than those attainable on earth can significantly advance applications in areas such as fiber optics communications, high power laser glasses, and other photonic devices where glasses are the key functional materials. The classical theories for nucleation and crystal growth for a glass or melt do not contain any parameter that is directly dependent upon the g-value, so it is not readily apparent why glasses prepared in microgravity should be more resistant to crystallization than equivalent glasses prepared on earth. Similarly, the gravity-driven convection in a fluid melt is believed to be the primary force field that is responsible for melt homogenization on earth. Thus, it is not obvious why a glass prepared in space, where gravity-driven convection is ideally absent, would be more chemically homogeneous than a glass identically prepared on earth. The primary objective of the present research is to obtain experimental data for the nucleation rate and crystal growth rate for a well characterized silicate melt (lithium disilicate) processed entirely in space (low gravity) and compare these rates with the nucleation and crystal growth rates for a similar glass prepared identically on earth (1g).

Day, Delbert E.↗

NASA NTRS1981

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.↗

NASA NTRS1988

The crystallization of tough thermoplastic resins in the presence of carbon fibers

The presence of carbon fibers increased the crystallization rates of both PEEK and PPS thermoplastic polymers. The effect was most pronounced at higher crystallization temperatures. Isothermal crystallization rates were analyzed by applying classical phenomenological nucleation theory. Unusually high values of the so-called Avrami exponent were found for neat PEEK. Isothermal crystallization of PEEK and PPS polymers produced crystalline samples having a wide variety of melting temperatures. The melting as observed by differential scanning calorimetry occurred as dual endotherms which were called primary (higher temperature) and secondary melting peaks. Each primary peak accounted for most of the crystallinity present. The secondary peaks represented the melting of crystallites formed later than those attributable to the primary endotherms. The presence of carbon fibers increased the thermal stability of both PEEK and PPS crystallites as manifested by higher temperatures for the primary melting peaks. This may be attributable to increased crystallite size, greater crystallite perfection, and/or favorable modification of the crystallite interface. Over the range studied, crystallization temperature strongly influenced the positions of the secondary peaks but not the primary peaks.

Theil, Michael H.↗

NASA NTRS1988

The critical complex in nucleation is not the nucleus

A theory of nucleation is presented which combines features of classical nucleation. In this theory, the nucleus is a cluster of finite size with a sharp interface and spinodal decomposition, in which a fluctuation in density or composition generates the critical complex and nucleus. Thus, the nucleus is a product of nucleation. Schematic models for the classical and the proposed routes to nucleation are compared, focusing on the relation between pressure and volume in the models. In the proposed model, the critical complex, or critical state, is between the parent state and the nucleus.

Rasmussen, Don H.↗

NASA NTRS1982

The effect of solute on the homogeneous crystal nucleation frequency in metallic melts

A complete calculation that extends the classical theory for crystal nucleation in pure melts to binary alloys has been made. Using a regular solution model, approximate expressions have been developed for the free energy change upon crystallization as a function of solute concentration. They are used, together with model-based estimates of the interfacial tension, to calculate the nucleation frequency. The predictions of the theory for the maximum attainable undercooling are compared with existing experimental results for non-glass forming alloys. The theory is also applied to several easy glass-forming alloys (Pd-Si, Au-Si, Fe-B) for qualitative comparison with the present experimental experience on the ease of glass formation, and for assessment of the potential for formation of the glass in bulk.

Thompson, C. V.↗

NASA NTRS1974

Cloud base levels for Jupiter and Venus and the heteromolecular nucleation theory

For purified binary gas mixtures like NH3-H2O or HCl-H2O, partial pressures appreciably greater than the two saturation partial pressures are needed to condense the gas mixture into small solution droplets (homogeneous heteromolecular nucleation). Thus without foreign nuclei, clouds are not as easily formed as in the theories of Lewis; the latter should be valid only if large condensation nuclei are available. We calculate here from classical homogeneous heteromolecular nucleation theory the threshold partial pressures necessary to achieve droplet nucleation for the gas mixtures NH3-H2O (Jupiter), HCl-H2O (Venus), H2SO4-H2O (Venus), and C2H5OH-H2O (laboratory).

Stauffer, D.↗

NASA NTRS1987

Combined homogeneous and heterogeneous crystal nucleation in glasses

The temperature dependence of combined homogeneous and heterogeneous crystal nucleation is examined within the framework of the classical theory. It is demonstrated that nucleation can have a local maximum rate at one or two temperatures. The physical parameters which cause large changes in the structure of the nucleation curve are elucidated. Also, the influence of saturation effects on the structure of nucleation curves is illustrated. The utilization of these results for the interpretation of experiments and for the production of controlled crystal nucleation in glass is considered.

Weinberg, Michael C.↗

NASA NTRS1983

Homogeneous crystal nucleation in binary metallic melts

A method for calculating the homogeneous crystal nucleation frequency in binary metallic melts is developed. The free energy of crystallization is derived from regular solution models for the liquid and solid and is used, together with model-based estimates of the interfacial tension, to calculate the nucleation frequency from the classical theory. The method can account for the composition dependence of the maximum undercooling observed in a number of experiments on small droplet dispersions. It can also be used to calculate the driving force for crystal growth and to obtain more precise estimates of the homogeneous crystal nucleation frequency in glass-forming alloys. This method, although approximate, is simple to apply, and requires only knowledge of the phase diagram and a few readily available thermodynamic quantities as input data.

Thompson, C. V.↗

NASA NTRS2002

Homogenous Surface Nucleation of Solid Polar Stratospheric Cloud Particles

A general surface nucleation rate theory is presented for the homogeneous freezing of crystalline germs on the surfaces of aqueous particles. While nucleation rates in a standard classical homogeneous freezing rate theory scale with volume, the rates in a surface-based theory scale with surface area. The theory is used to convert volume-based information on laboratory freezing rates (in units of cu cm, seconds) of nitric acid trihydrate (NAT) and nitric acid dihydrate (NAD) aerosols into surface-based values (in units of sq cm, seconds). We show that a surface-based model is capable of reproducing measured nucleation rates of NAT and NAD aerosols from concentrated aqueous HNO3 solutions in the temperature range of 165 to 205 K. Laboratory measured nucleation rates are used to derive free energies for NAT and NAD germ formation in the stratosphere. NAD germ free energies range from about 23 to 26 kcal mole, allowing for fast and efficient homogeneous NAD particle production in the stratosphere. However, NAT germ formation energies are large (greater than 26 kcal mole) enough to prevent efficient NAT particle production in the stratosphere. We show that the atmospheric NAD particle production rates based on the surface rate theory are roughly 2 orders of magnitude larger than those obtained from a standard volume-based rate theory. Atmospheric volume and surface production of NAD particles will nearly cease in the stratosphere when denitrification in the air exceeds 40 and 78%, respectively. We show that a surface-based (volume-based) homogeneous freezing rate theory gives particle production rates, which are (not) consistent with both laboratory and atmospheric data on the nucleation of solid polar stratospheric cloud particles.

Tabazadeh, A.↗

NASA NTRS2008

Understanding Ice Supersaturation, Particle Growth, and Number Concentration in Cirrus Clouds

Many factors control the ice supersaturation and microphysical properties in cirrus clouds. We explore the effects of dynamic forcing, ice nucleation mechanisms, and ice crystal growth rate on the evolution and distribution of water vapor and cloud properties in nighttime cirrus clouds using a one-dimensional cloud model with bin microphysics and remote sensing measurements obtained at the Department of Energy's Atmospheric Radiation Measurement (ARM) Climate Research Facility located near Lamont, OK. We forced the model using both large-scale vertical ascent and, for the first time, mean mesoscale velocity derived from radar Doppler velocity measurements. Both heterogeneous and homogeneous nucleation processes are explored, where a classical theory heterogeneous scheme is compared with empirical representations. We evaluated model simulations by examining both bulk cloud properties and distributions of measured radar reflectivity, lidar extinction, and water vapor profiles, as well as retrieved cloud microphysical properties. Our results suggest that mesoscale variability is the primary mechanism needed to reproduce observed quantities. Model sensitivity to the ice growth rate is also investigated. The most realistic simulations as compared with observations are forced using mesoscale waves, include fast ice crystal growth, and initiate ice by either homogeneous or heterogeneous nucleation. Simulated ice crystal number concentrations (tens to hundreds particles per liter) are typically two orders of magnitude smaller than previously published results based on aircraft measurements in cirrus clouds, although higher concentrations are possible in isolated pockets within the nucleation zone.

Comstock, Jennifer M.↗