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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.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Ion irradiation induced nucleation and growth of nanoparticles in amorphous silicon carbide at elevated temperatures

Ion irradiation induced crystallization in as-deposited amorphous SiC films is investigated using grazing-angle incidence x-ray diffraction (GIXRD), transmission electron microscopy (TEM) and Raman spectroscopy. Irradiation with 5 MeV Xe to fluence of 115 Xe/nm2 at 700 K results in a homogenous distribution of 3C-SiC grains with an average crystallite size of ~5.7 nm over the entire film thickness (~1 µm). The nucleation and growth processes exhibit a weak dependence on dose in displacements per atom (dpa) in the dose range from 6 to 20 dpa. A transformation of homonuclear C-C bonds from sp3 to sp2 hybridization is observed in the irradiated films, which may be partly responsible for the observed grain size saturation. The results from this study may have a significant impact on synthesis of nanograins in amorphous SiC and other similar materials with effective control of grain size and density by ion irradiation.

phase transformation, SiC, ion irradiation↗
DOE OSTI2020

Recent experimental explorations of non-classical nucleation

Nucleation, the early stage of crystallization, is a key step in producing functional materials, but nucleation processes have yet to be understood in detail. Recent advanced characterization techniques, especially atomic force microscopy, liquid-cell transmission electron microscopy (TEM) and cryo-TEM, enable scientists to observe previously inaccessible nucleation details at the nanoscale. In this review, we summarize newly suggested non-classical nucleation models with respect to mechanistic understanding from experimental views, which highlight multi-step nucleation mechanisms. Different intermediated phases such as clusters at the pre-nucleation stage, liquid-like precursors, amorphous phases and even oligomers have been revealed, which play vital roles in nucleation and structure control. Moreover, these intermediated phases practically contribute in general to the structural variances of materials for nanoscience and nanotechnology. Overall, these studies ultimately enable us to control nucleation processes for materials synthesis.

Jin, Biao↗
DOE OSTI2018

Control of Calcium Phosphate Nucleation and Transformation through Interactions of Enamelin and Amelogenin Exhibits the “Goldilocks Effect”

Although amelogenin comprises the vast majority of the matrix that templates calcium phosphate nucleation during enamel formation, other proteins, particularly enamelin, are also known to play an important role in the formation of enamel’s intricate architecture. However, there is little understanding of the interplay between amelogenin and enamelin in controlling processes of mineral nucleation and growth. Here we used an in vitro model to investigate the impact of enamelin co-assembly with amelogenin on calcium phosphate nucleation for a range of enamelin-to-amelogenin ratios. We found that amelogenin alone is a weak promoter of nucleation, but addition of enamelin enhanced nucleation rates in a highly non-linear, non-monotonic manner reaching a sharp maximum at a ratio of 1:50. We provide a phenomenological model to explain this effect that assumes only isolated enamelin proteins can act as sites of enhanced nucleation, while enamelin oligomers cannot. Even when co-assembly is random, the model reproduces the observed behavior, suggesting a simple means to tightly control the timing and extent of nucleation and phase transformation by amelogenin and enamelin.

Tao, Jinhui↗
DOE OSTI2019

Organic-Mineral Interfacial Chemistry Drives Heterogeneous Nucleation of Sr-Rich (Bax, Sr1-x)SO4 from Undersaturated Solution

Sr-bearing marine barite [(Bax, Sr1-x)SO4] cycling has been widely used to reconstruct geochemical evolutions of paleoenvironments. However, an understanding of barite precipitation in the ocean, which is globally undersaturated with respect to barite, is missing. Moreover, the reason for the occurrence of higher Sr content in marine barites than expected for classical crystal growth processes remains unknown. Field data analyses suggested that organic molecules may regulate the formation and composition of marine barites; however, the specific organic–mineral interactions are unclear. Using in situ grazing incidence small-angle X-ray scattering (GISAXS), size and total volume evolutions of barite precipitates on organic films were characterized. The results show that barite forms on organic films from undersaturated solutions. Moreover, from a single supersaturated solution with respect to barite, Sr-rich barite nanoparticles formed on organics, while micrometer-size Sr-poor barites formed in bulk solutions. Ion adsorption experiments showed that organic films can enrich cation concentrations in the adjacent solution, thus increasing the local supersaturation and promoting barite nucleation on organic films, even when the bulk solution was undersaturated. The Sr enrichment in barites formed on organic films was found to be controlled by solid-solution nucleation rates; instead, the Sr-poor barite formation in bulk solution was found to be controlled by solid-solution growth rates. This study provides a mechanistic explanation for Sr-rich marine barite formation and offers insights for understanding and controlling the compositions of solid solutions by separately tuning their nucleation and growth rates via the unique chemistry of solution–organic interfaces.

Deng, Ning↗
DOE OSTI2025

A stress-sensitive precipitate nucleation model beyond classical nucleation theory

The dynamic evolution of precipitates and second phases dictates the strength and stability of most engineering alloys. By design, or as a consequence of thermo-mechanical aging, engineering metals and alloys often form precipitates of second phases when subjecting to diverse thermal and mechanical loads. Precipitation is governed by several factors, including the alloy’s composition, processing/operating temperature, and stresses — either as a result of external loads or from residual stresses. However, state-of-the-art models for precipitate nucleation (i.e., classical nucleation theory) typically lacks consistent method to capture the effects of externally applied and/or internal stresses on nucleation; thereby severely limiting the applicability of these models to complex materials systems and to representative loading scenarios. Here, in this work, we extend upon classical nucleation theory to account for the effect of stresses on precipitation kinetics and thermodynamics. This is achieved via the use of an Eshelbian micromechanics framework keeping track of (i) the stress build up resulting from second phase formation as a function of mechanical load and, (ii) the effects of dislocations on precipitate formation. This new model is applied to σ precipitate in Fe–Cr binary alloys and M 23 C 6 precipitate in 316H stainless steel (SS). Simulations demonstrate the important role of both the remotely applied loads and dislocation pile ups on precipitate nucleation.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Nucleation and phase transformation pathways in electrolyte solutions investigated by in situ microscopy techniques

Identification of crystal nucleation and growth pathways is of fundamental importance for synthesis of functional materials, which requires control over size, orientation, polymorph, and hierarchical structure, often in the presence of additives used to tune the energy landscape defining these pathways. Furthermore we summarize the recent progress in application of in situ TEM and AFM techniques to monitor or even tune the pathway of crystal nucleation and growth.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Two-level systems in nucleated and non-nucleated epitaxial alpha-tantalum films

Building usefully coherent superconducting quantum processors depends on reducing losses in their constituent materials. Tantalum, like niobium, has proven utility as the primary superconducting layer within highly coherent qubits. However, unlike Nb, high temperatures are typically used to stabilize the desirable body-centered-cubic phase, α-Ta, during thin film deposition. It has long been known that a thin Nb layer permits the room-temperature nucleation of α-Ta, but here we observe the epitaxial process and present few-photon microwave loss measurements in Nb-nucleated Ta films. We compare resonators patterned from Ta films grown at high temperature (500 °C) and films nucleated at room temperature, in order to understand the impact of the crystalline order on quantum coherence. In both cases, films grew with Al 2 O 3 (001) ∥ Ta (110), indicating that the epitaxial orientation is independent of temperature and is preserved across the Nb/Ta interface. We use conventional low-power spectroscopy to measure two level system (TLS) loss as well as an electric-field bias technique to measure the effective dipole moments of TLS in the surfaces of resonators. In our measurements, Nb-nucleated Ta resonators had greater loss tangent (1.5 ± 0.1 × 10 -5 ) than non-nucleated (5 ± 1× 10 -6 ) in approximate proportion to defect densities as characterized by x-ray diffraction (0.27° vs 0.18° [110] reflection width) and electron microscopy (30 vs 70 nm domain size). Furthermore, the dependence of the loss tangent on domain size indicates that the development of more ordered Ta films is likely to lead to improvements in qubit coherence times. Moreover, low-temperature α-Ta epitaxy may enable the growth of microstate-free heterostructures, which would not withstand high temperature processing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Field intercomparison of ice nucleation measurements: the Fifth International Workshop on Ice Nucleation Phase 3 (FIN-03)

Abstract. The third phase of the Fifth International Ice Nucleation Workshop (FIN-03) was conducted at the Storm Peak Laboratory in Steamboat Springs, Colorado, in September 2015 to facilitate the intercomparison of instruments measuring ice-nucleating particles (INPs) in the field. Instruments included two online and four offline measurement systems for INPs, which are a subset of those utilized in the laboratory study that comprised the second phase of FIN (FIN-02). The composition of the total aerosols was characterized using the Particle Analysis by Laser Mass Spectrometry (PALMS) and Wideband Integrated Bioaerosol Sensor (WIBS) instruments, and aerosol size distributions were measured by a laser aerosol spectrometer (LAS). The dominant total particle compositions present during FIN-03 were composed of sulfates, organic compounds, and nitrates, as well as particles derived from biomass burning. Mineral-dust-containing particles were ubiquitous throughout and represented 67 % of supermicron particles. Total WIBS fluorescing particle concentrations for particles with diameters of > 0.5 µm were 0.04 ± 0.02 cm−3 (0.1 cm−3 highest; 0.02 cm−3 lowest), typical of the warm season in this region and representing ≈ 9 % of all particles in this size range as a campaign average. The primary focus of FIN-03 was the measurement of INP concentrations via immersion freezing at temperatures > −33 °C. Additionally, some measurements were made in the deposition nucleation regime at these same temperatures, representing one of the first efforts to include both mechanisms within a field campaign. INP concentrations via immersion freezing agreed within factors ranging from nearly 1 to 5 times on average between matched (time and temperature) measurements, and disagreements only rarely exceeded 1 order of magnitude for sampling times coordinated to within 3 h. Comparisons were restricted to temperatures lower than −15 °C due to the limits of detection related to sample volumes and very low INP concentrations. Outliers of up to 2 orders of magnitude occurred between −25 and −18 °C; a better agreement was seen at higher and lower temperatures. Although the 5–10 factor agreement of INP measurements found in FIN-03 aligned with the results of the FIN-02 laboratory comparison phase, giving confidence in progress of this measurement field, this level of agreement still equates to temperature uncertainties of 3.5 to 5 °C that may not be sufficient for numerical cloud modeling applications that utilize INP information. INP activity in the immersion-freezing mode was generally found to be an order of magnitude or more, making it more efficient than in the deposition regime at 95 %–99 % water relative humidity, although this limited data set should be augmented in future efforts. To contextualize the study results, an assessment was made of the composition of INPs during the late-summer to early-fall period of this study inferred through comparison to existing ice nucleation parameterizations and through measurement of the influence of thermal and organic carbon digestion treatments on immersion-freezing ice nucleation activity. Consistent with other studies in continental regions, biological INPs dominated at temperatures of > −20 °C and sometimes colder, while arable dust-like or other organic-influenced INPs were inferred to dominate below −20 °C.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Toward Automated Sampling of Polymorph Nucleation and Free Energies with the SGOOP and Metadynamics

Understanding the driving forces behind the nucleation of different polymorphs is of great importance for material sciences and the pharmaceutical industry. This includes understanding the reaction coordinate that governs the nucleation process and correctly calculating the relative free energies of different polymorphs. Here, we demonstrate, for the prototypical case of urea nucleation from the melt, how one can learn such a one-dimensional reaction coordinate as a function of prespecified order parameters and use it to perform efficient biased all-atom molecular dynamics simulations. The reaction coordinate is learnt as a function of the generic thermodynamic and structural order parameters using the “spectral gap optimization of order parameters (SGOOP)” approach [Tiwary, P. and Berne, B. J. Proc. Natl. Acad. Sci. U.S.A. (2016)] and is biased using well-tempered metadynamics simulations. The reaction coordinate gives insights into the role played by different structural and thermodynamics order parameters, and the biased simulations obtain accurate relative free energies for different polymorphs. This includes an accurate prediction of the approximate pressure at which urea undergoes a phase transition and one of the metastable polymorphs becomes the most stable conformation. Here, we believe the ideas demonstrated in this work will facilitate efficient sampling of nucleation in complex, generic systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Enhanced Stability of Li Metal Anodes by Synergetic Control of Nucleation and the Solid Electrolyte Interphase

Use of a protective coating on a lithium (Li) metal anode (LMA) is an effective approach to enhance its coulombic efficiency and cycling stability. Here we report a facile approach to produce uniform silver (Ag) nanoparticle-decorated LMAs for high-performance Li metal batteries (LMBs). This effective treatment can lead to well controlled nucleation and the formation of a stable solid electrolyte interphase (SEI). Ag nanoparticles embedded in the surface of Li anodes induced uniform Li plating/stripping morphologies with reduced overpotential. More importantly, cross-linked lithium fluoride (LiF) networks formed during Ag+ reduction enabled a highly stable SEI layer. Based on the Ag-LiF decorated anodes, LMBs with LiNi1/3Mn1/3Co1/3O2 cathode (~1.8 mAh cm-2) can retain >80% capacity over 500 cycles. The similar results were also obtained when the same approach was applied to the design of stable sodium (Na) anodes. These results indicate that synergetic control of the nucleation and SEI is an efficient approach to stabilize rechargeable metal batteries.

anode↗
DOE OSTI2020

Precipitation-site competition in duplex stainless steels: Cu clusters vs spinodal decomposition interfaces as nucleation sites during thermal aging

Competing microstructural evolution mechanisms can exist simultaneously when duplex stainless steels are operating for several decades in a high temperature service environment. Such competition between different microstructural evolution pathways can be difficult to ascertain using simple model alloy systems necessitating detailed structural and compositional analysis of phase transformation mechanisms in complex alloys Thus, in this study duplex stainless steels with complex but well understood chemistries were used to investigate the relative importance of different heterogeneous nucleation sites – specifically spinodal decomposition and Cu clustering – on precipitation of Ni-Si-Mn particles during long term thermal aging. Precipitation of Ni-Si-Mn particles in duplex stainless steels and ferritic steels during thermal aging and irradiation is known to have profound effect on mechanical properties. Using duplex stainless steels with custom modified compositions along with atom probe tomography characterization and first-passage kinetic Monte Carlo (FPKMC) simulations it is revealed that while the interface between Cr and Fe formed during spinodal decomposition can be a pathway for diffusion of Ni, Si, Mn, and Cu, it is not a site that encourages precipitation of Ni-Si-Mn rich particles. Instead, the presence of a higher concentration of Cu in these steels leads to formation of small Cu clusters with high energy interfaces that act as nucleation sites for Ni-Si-Mn particles because of its strong interaction particularly with Ni increasing the chemical driving force for precipitation. These results will help inform predictive models for the use of duplex stainless steels and other precipitation-hardened alloys for extended operation at high temperatures.

Duplex stainless steel, Thermal aging, Precipitati↗
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↗