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All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements

Abstract. The second phase of the Fifth International Ice Nucleation Workshop (FIN-02)involved the gathering of a large number of researchers at the KarlsruheInstitute of Technology's Aerosol Interactions and Dynamics of the Atmosphere(AIDA) facility to promote characterization and understanding of icenucleation measurements made by a variety of methods used worldwide.Compared to the previous workshop in 2007, participation was doubled,reflecting a vibrant research area. Experimental methods involved sampling ofaerosol particles by direct processing ice nucleation measuring systems fromthe same volume of air in separate experiments using different ice nucleatingparticle (INP) types, and collections of aerosol particle samples ontofilters or into liquid for sharing amongst measurement techniques thatpost-process these samples. In this manner, any errors introduced bydifferences in generation methods when samples are shared across laboratorieswere mitigated. Furthermore, as much as possible, aerosol particle sizedistribution was controlled so that the size limitations of different methodswere minimized. The results presented here use data from the workshop toassess the comparability of immersion freezing measurement methods activatingINPs in bulk suspensions, methods that activate INPs in condensation and/orimmersion freezing modes as single particles on a substrate, continuous flowdiffusion chambers (CFDCs) directly sampling and processing particles wellabove water saturation to maximize immersion and subsequent freezing ofaerosol particles, and expansion cloud chamber simulations in which liquidcloud droplets were first activated on aerosol particles prior to freezing.The AIDA expansion chamber measurements are expected to be the closestrepresentation to INP activation in atmospheric cloud parcels in thesecomparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX andpotassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam(Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively,and a bacterial INP (Snomax ® ). Consideredtogether, the agreement among post-processed immersion freezing measurementsof the numbers and fractions of particles active at different temperaturesfollowing bulk collection of particles into liquid was excellent, withpossible temperature uncertainties inferred to be a key factor in determiningINP uncertainties. Collection onto filters for rinsing versus directly intoliquid in impingers made little difference. For methods that activatedcollected single particles on a substrate at a controlled humidity at orabove water saturation, agreement with immersion freezing methods was good inmost cases, but was biased low in a few others for reasons that have not beenresolved, but could relate to water vapor competition effects. AmongstCFDC-style instruments, various factors requiring (variable) highersupersaturations to achieve equivalent immersion freezing activation dominatethe uncertainty between these measurements, and for comparison with bulkimmersion freezing methods. When operated above water saturation to includeassessment of immersion freezing, CFDC measurements often measured at orabove the upper bound of immersion freezing device measurements, but oftenunderestimated INP concentration in comparison to an immersion freezingmethod that first activates all particles into liquid droplets prior tocooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber–Portable Ice Nucleation Chamber), and typically slightly underestimated INPnumber concentrations in comparison to cloud parcel expansions in the AIDAchamber; this can be largely mitigated when it is possible to raise therelative humidity to sufficiently high values in the CFDCs, although this isnot always possible operationally. Correspondence of measurements of INPs among direct sampling andpost-processing systems varied depending on the INP type. Agreement was bestfor Snomax ® particles in the temperature regimecolder than −10 ∘ C, where their ice nucleation activity is nearlymaximized and changes very little with temperature. At temperatures warmer than −10 ∘ C, Snomax ® INP measurements (allvia freezing of suspensions) demonstrated discrepancies consistent withprevious reports of the instability of its protein aggregates that appear tomake it less suitable as a calibration INP at these temperatures. ForArgentinian soil dust particles, there was excellent agreement across allmeasurement methods; measures ranged within 1 order of magnitude for INPnumber concentrations, active fractions and calculated active site densitiesover a 25 to 30 ∘ C range and 5 to 8 orders of correspondingmagnitude change in number concentrations. This was also the case for alltemperatures warmer than −25 ∘ C in Tunisian dust experiments. Incontrast, discrepancies in measurements of INP concentrations or active sitedensities that exceeded 2 orders of magnitude across a broad range of temperaturemeasurements found at temperatures warmer than −25 ∘ C in a previous study werereplicated for illite NX. Discrepancies also exceeded 2 orders of magnitude attemperatures of −20 to −25 ∘ C for potassium feldspar (K-feldspar), but these coincidedwith the range of temperatures at which INP concentrations increase rapidly atapproximately an order of magnitude per 2 ∘ C cooling forK-feldspar. These few discrepancies did not outweigh the overall positive outcomes of theworkshop activity, nor the future utility of this data set or future similarefforts for resolving remaining measurement issues. Measurements of the samematerials were repeatable over the time of the workshop and demonstratedstrong consistency with prior studies, as reflected by agreement of databroadly with parameterizations of different specific or general (e.g., soildust) aerosol types. The divergent measurements of the INP activity of illiteNX by direct versus post-processing methods were not repeated for otherparticle types, and the Snomax ® datademonstrated that, at least for a biological INP type, there is no expectedmeasurement bias between bulk collection and direct immediately processedfreezing methods to as warm as −10 ∘ C. Since particle size rangeswere limited for this workshop, it can be expected that for atmosphericpopulations of INPs, measurement discrepancies will appear due to thedifferent capabilities of methods for sampling the full aerosol sizedistribution, or due to limitations on achieving sufficient watersupersaturations to fully capture immersion freezing in direct processinginstruments. Overall, this workshop presents an improved picture of presentcapabilities for measuring INPs than in past workshops, and providesdirection toward addressing remaining measurement issues.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

The Portable Ice Nucleation Experiment (PINE): a new online instrument for laboratory studies and automated long-term field observations of ice-nucleating particles

Atmospheric ice-nucleating particles (INPs) play an important role in determining the phase of clouds, which affects their albedo and lifetime. A lack of data on the spatial and temporal variation of INPs around the globe limits our predictive capacity and understanding of clouds containing ice. Automated instrumentation that can robustly measure INP concentrations across the full range of tropospheric temperatures is needed in order to address this knowledge gap. In this study, we demonstrate the functionality and capacity of the new Portable Ice Nucleation Experiment (PINE) to study ice nucleation processes and to measure INP concentrations under conditions pertinent for mixed-phase clouds, with temperatures from about -10 to about -40°C. PINE is a cloud expansion chamber which avoids frost formation on the cold walls and thereby omits frost fragmentation and related background ice signals during the operation. The development, working principle and treatment of data for the PINE instrument is discussed in detail. We present laboratory-based tests where PINE measurements were compared with those from the established AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber. Within experimental uncertainties, PINE agreed with AIDA for homogeneous freezing of pure water droplets and the immersion freezing activity of mineral aerosols. Results from a first field campaign conducted at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) observatory in Oklahoma, USA, from 1 October to 14 November 2019 with the latest PINE design (a commercially available PINE chamber) are also shown, demonstrating PINE's ability to make automated field measurements of INP concentrations at a time resolution of about 8 min with continuous temperature scans for INP measurements between -10 and -30°C. During this field campaign, PINE was continuously operated for 45 d in a fully automated and semi-autonomous way, demonstrating the capability of this new instrument to also be used for longer-term field measurements and INP monitoring activities in observatories.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2011

Orientation and Morphology of Calcite Nucleated under Floating Monolayers: A Magnesium-ion-enhanced Nucleation Study

We have studied the biomimetic growth of calcium carbonate crystals under floating monolayer templates, in the presence of Mg ions, using grazing incidence X-ray diffraction and SEM imaging. Crystals grown under sulfate monolayers nucleate from the (0 0 1) plane with and without Mg ions, while undergoing substantial changes in morphology. Crystals grown under alcohol monolayers nucleate from the (1 0 4) plane in the presence of Mg. X-ray data do not detect orientation in crystals grown under acid monolayers, but at higher Mg concentrations the resulting morphologies are indicative of template-nucleated growth. These results suggest that Mg provides living organisms a way to enhance the orientation and control the morphology of acid-templated crystals.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Inclusion of line tension effect in classical nucleation theory for heterogeneous nucleation: A rigorous thermodynamic formulation and some unique conclusions

A rigorous thermodynamic formulation of the geometric model for heterogeneous nucleation including line tension effect is missing till date due to the associated mathematical hurdles. In this work, we develop a novel thermodynamic formulation based on Classical Nucleation Theory (CNT), which is supposed to illustrate a systematic and a more plausible analysis for the heterogeneous nucleation on a planar surface including the line tension effect. The appreciable range of the critical microscopic contact angle (θ{sub c}), obtained from the generalized Young’s equation and the stability analysis, is θ{sub ∞} < θ{sub c} < θ′ for positive line tension and is θ{sub M} < θ{sub c} < θ{sub ∞} for negative line tension. θ{sub ∞} is the macroscopic contact angle, θ′ is the contact angle for which the Helmholtz free energy has the minimum value for the positive line tension, and θ{sub M} is the local minima of the nondimensional line tension effect for the negative line tension. The shape factor f, which is basically the dimensionless critical free energy barrier, becomes higher for lower values of θ{sub ∞} and higher values of θ{sub c} for positive line tension. The combined effect due to the presence of the triple line and the interfacial areas (f{sup L} + f{sup S}) in shape factor is always within (0, 3.2), resulting f in the range of (0, 1.7) for positive line tension. A formerly presumed appreciable range for θ{sub c}(0 < θ{sub c} < θ{sub ∞}) is found not to be true when the effect of negative line tension is considered for CNT. Estimation based on the property values of some real fluids confirms the relevance of the present analysis.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Demonstration of neutron radiation-induced nucleation of supercooled water

In this study, we present direct evidence for neutrons causing nucleation of supercooled water. Highly purified water (20 nm filtration) is cooled to well below freezing (as low as −20 °C) with a radioactive calibration source of neutrons/gamma-rays either present or removed during each of many control cooling runs for the same volume of water. When it is primarily neutrons irradiating the sample bulk, the non-equilibrium freezing point (also known as the “supercooling point”) is, on average, +0.7 °C warmer than the control equivalent, with a statistical significance of greater than 5 Sigma, with systematic uncertainty included. This effect is not observed with water in the presence of gamma-rays instead of neutrons. While these neutrons should have theoretically had sufficient energy to mount the energy barrier, corroborating our results, their raising of supercooling temperature has never been reported experimentally to the best of our knowledge. The potential to use deeply supercooled solutions, not only water, as metastable detectors for radiation and perhaps dark matter or neutrino physics presents now a new avenue for exploration.

Szydagis, Matthew↗
NASA NTRS1990

The effect of multiple nucleation events on heterogeneous nucleation rates

The effect of multiple nucleation events on the overall heterogeneous nucleation rate is studied using a simple model based on coupled consecutive chemical reactions. It is found that the decay of the nucleation curve and the saturation time depend on the maximum number of nuclei which can be accomodated on a particle.

Weinberg, Michael C.↗
NASA NTRS2000

The Effects of Thermal History on Nucleation of Tetragonal Lysozyme Crystals, or Hot Protein and Cold Nucleation

Chicken egg white lysozyme has a well characterized thermally driven phase transition. Between pH 4.2 and 5.2, the transition temperature, as defined by the point where the tetragonal and orthorhombic solubilities are equal, is a function of the pH, salt (precipitant) type and concentration, and most likely of the buffer concentration as well. This phase transition can be carried out with protein solution alone, prior to addition of precipitant solution. Warming a lysozyme solution above the phase transition point, then cooling it back below this point, has been shown to affect the subsequent nucleation rate, as determined by the numbers and size of crystals formed, but not the growth rate for the tetragonal crystal form . We have now measured the kinetics of this process and investigated its reversibility. The transition effects are progressive with temperature, having a half time of about 1 hour at 37C at pH 4.8. After holding a lysozyme solution at 37C (prior to addition of precipitant) for 16 hours, then cooling it back to 4C no return to the pre-warmed nucleation kinetics are observed after at least 4 weeks. Orthorhombic lysozyme crystals apparently do not undergo the flow-induced growth cessation of tetragonal lysozyme crystals. Putting the protein in the orthorhombic form does not affect the averaged face growth kinetics, only nucleation, for tetragonal crystals. This differential behaviour may be exploited to elucidate how and where flow affects the lysozyme crystal growth process. The presentation will focus on the results of these and ongoing studies in this area.

Burke, Michael↗
DOE OSTI2013

Numerical Studies of Nucleation and Bubble Growth in Thermoplastic Foams at high Nucleation Rates

The influence volume approach (IVA) provides a coherent way of modeling the simultaneous nucleation and bubble growth during the foaming of thermoplastic polymers. In this work, a numerical model based on the influence volume approach is used to investigate the path to creating thermoplastic foams with nano-cellular structure. In particular, the diffusion of the blowing agent inside the polymer during the initial nucleation and later during bubble growth is analyzed. It is found that as the depressurization rate increases the gas diffusion becomes the limiting factor for bubble growth allowing for greater number of nuclei to be formed. However after a critical value of depressurization rate, further increase in depressurization rate appears to have no effect on the final bubble diameter. We comment on this critical depressurization rate based on classical nucleation theory.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Competitive B2 and B33 Nucleation during Solidification of Ni 50 Zr 50 Alloy: Molecular Dynamics Simulation and Classical Nucleation Theory

We studied the homogenous nucleation of the stoichiometric B2 and B33 phases in the Ni 50 Zr 50 alloy using the persistent embryo method and the classical nucleation theory. The two phases become very close competitors at large supercoolings, which is consistent with the experimental observations. In the case of the B2 phase, the linear temperature dependence of the solid–liquid interface (SLI) free energy extrapolated to the melting temperature leads to the same value as the one obtained from the capillarity fluctuation method (CFM). In the case of the B33 phases, the SLI free energy is also a linear function of temperature at large supercoolings, but the extrapolation to the melting temperature leads to a value which is considerably different from the CFM value. This is persistent with the large anisotropy of the SLI properties of the B33 phase nearby the melting temperature observed in the simulation of the nominally flat interface migration.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Countercations Control Local Specific Bonding Interactions and Nucleation Mechanisms in Concentrated Water-in-Salt Solutions

One of the continuing challenges presented in aqueous salt solutions is to understand ion association reactions driving dynamic demixing from solvation, complexation and solute clustering. The problems understanding this phenomenon are exacerbated in the highly-concentrated water-in-salt electrolytes, where the deficiency of water leads to a dramatic retardation of solvating water and formation of extended solvent-solute clustering networks. By probing microscopic dynamics of water and prenucleation clusters using quasi-elastic neutron scattering and proton nuclear magnetic resonance spectroscopy, we observed contrasting mechanistic specifics of ion-water mobilities in highly-concentrated Na+- vs. K+-based aluminate solutions (diffusion coefficients of 0.2 vs. 2.6?10-10m2s-1 at 293 K, respectively). The magnitude of the differences is far beyond the kosmotropic (Na+) and chaotropic (K+) effects typically understood at low ionic concentrations. The distinct crystallization mechanisms observed in analogous deuterated systems further imply that different prenucleation cluster dynamics and network packing morphologies can either frustrate or promote crystallization, as described by non-classical nucleation theory.

Wang, Hsiu-Wen↗
DOE OSTI2015

Molecular simulations of heterogeneous ice nucleation. I. Controlling ice nucleation through surface hydrophilicity

Ice formation is one of the most common and important processes on earth and almost always occurs at the surface of a material. A basic understanding of how the physicochemical properties of a material’s surface affect its ability to form ice has remained elusive. Here, we use molecular dynamics simulations to directly probe heterogeneous ice nucleation at a hexagonal surface of a nanoparticle of varying hydrophilicity. Surprisingly, we find that structurally identical surfaces can both inhibit and promote ice formation and analogous to a chemical catalyst, it is found that an optimal interaction between the surface and the water exists for promoting ice nucleation.We use our microscopic understanding of the mechanism to design a modified surface in silico with enhanced ice nucleating ability. C 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.

Cox, Stephen J.↗