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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 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Nucleation and growth of Nb nanoclusters during plasma gas condensation

Niobium nanoclusters were produced using a plasma gas condensation process. The influence of gas flow rate, aggregation length, and source current on the nanocluster nucleation and growth were analyzed. Nanoclusters with an average diameter from 4 nm to 10 nm were produced. Cluster size and concentration were tuned by controlling the process inputs. The effects of each parameter on the nucleation zone, growth length, and residence time was examined. The parameters do not affect the cluster formation and growth independently; their influence on cluster formation can be either cumulative or competing. Examining the nucleation and growth over a wide combination of parameters provided insight into their interactions and the impact on the growth process. These results provide the opportunity for a broader understanding into the nucleation and growth of nanoclusters and some insights into how process parameters interact during deposition. This knowledge will enhance the ability to create nanoclusters with desired size dispersions.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Direct measurement of activation time and nucleation rate in capillary-condensed water nanomeniscus

We demonstrate real-time observation of nucleation of the single water nanomeniscus formed via capillary condensation. We directly measure (i) activation time by time-resolved atomic force microscopy and (ii) nucleation rate by statistical analysis of its exponential distribution, which is the experimental evidence that the activation process is stochastic and follows the Poisson statistics. It implies that formation of the water nanomeniscus is triggered by nucleation, which requires activation for producing a nucleus. We also find the dependence of the nucleation rate on the tip-sample distance and temperature.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Kinetics of self-induced nucleation and optical properties of GaN nanowires grown by plasma-assisted molecular beam epitaxy on amorphous Al{sub x}O{sub y}

Nucleation kinetics of GaN nanowires (NWs) by molecular beam epitaxy on amorphous Al{sub x}O{sub y} buffers deposited at low temperature by atomic layer deposition is analyzed. We found that the growth processes on a-Al{sub x}O{sub y} are very similar to those observed on standard Si(111) substrates, although the presence of the buffer significantly enhances nucleation rate of GaN NWs, which we attribute to a microstructure of the buffer. The nucleation rate was studied vs. the growth temperature in the range of 720–790 °C, which allowed determination of nucleation energy of the NWs on a-Al{sub x}O{sub y} equal to 6 eV. This value is smaller than 10.2 eV we found under the same conditions on nitridized Si(111) substrates. Optical properties of GaN NWs on a-Al{sub x}O{sub y} are analyzed as a function of the growth temperature and compared with those on Si(111) substrates. A significant increase of photoluminescence intensity and much longer PL decay times, close to those on silicon substrates, are found for NWs grown at the highest temperature proving their high quality. The samples grown at high temperature have very narrow PL lines. This allowed observation that positions of donor-bound exciton PL line in the NWs grown on a-Al{sub x}O{sub y} are regularly lower than in samples grown directly on silicon suggesting that oxygen, instead of silicon, is the dominant donor. Moreover, PL spectra suggest that total concentration of donors in GaN NWs grown on a-Al{sub x}O{sub y} is lower than in those grown under similar conditions on bare Si. This shows that the a-Al{sub x}O{sub y} buffer efficiently acts as a barrier preventing uptake of silicon from the substrate to GaN.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Effect of inter-species selective interactions on the thermodynamics and nucleation free-energy barriers of a tessellating polyhedral compound

The phase behavior and the homogeneous nucleation of an equimolar mixture of octahedra and cuboctahedra are studied using thermodynamic integration, Gibbs-Duhem integration, and umbrella sampling simulations. The components of this mixture are modeled as polybead objects of equal edge lengths so that they can assemble into a space-filling compound with the CsCl crystal structure. Taking as reference the hard-core system where the compound crystal does not spontaneously nucleate, we quantified the effect of inter-species selective interactions on facilitating the disorder-to-order transition. Facet selective and facet non-selective inter-species attractions were considered, and while the former was expectedly more favorable toward the target tessellating structure, the latter was found to be similarly effective in nucleating the crystal compound. Ranges for the strength of attractions and degree of supersaturation were identified where the nucleation free-energy barrier was small enough to foretell a fast process but large enough to prevent spinodal fluctuations that can trap the system in dense metastable states lacking long-range order. At those favorable conditions, the tendency toward the local orientational order favored by packing entropy is amplified and found to play a key role seeding nuclei with the CsCl structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Modelling the effect of acoustic waves on nucleation

A phase transformation in a metastable phase can be affected when it is subjected to a high intensity ultrasound wave. In this study we determined the effect of oscillation in pressure and temperature on a phase transformation using the Gibbs droplet model in a generic format. The developed model is valid for both equilibrium and non-equilibrium clusters formed through a stationary or non-stationary process. We validated the underlying model by comparing the predicted kinetics of water droplet formation from the gas phase against experimental data in the absence of ultrasound. Our results demonstrated better agreement with experimental data in comparison with classical nucleation theory. Then, we determined the thermodynamics and kinetics of nucleation and the early stage of growth of clusters in an isothermal sonocrystallisation process. This new contribution shows that the effect of pressure on the kinetics of nucleation is cluster size-dependent in contrast to classical nucleation theory.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Driving and characterizing nucleation of urea and glycine polymorphs in water

Crystal nucleation is relevant across the domains of fundamental and applied sciences. However, in many cases, its mechanism remains unclear due to a lack of temporal or spatial resolution. To gain insights into the molecular details of nucleation, some form of molecular dynamics simulations is typically performed; these simulations, in turn, are limited by their ability to run long enough to sample the nucleation event thoroughly. To overcome the timescale limits in typical molecular dynamics simulations in a manner free of prior human bias, here, we employ the machine learning-augmented molecular dynamics framework “reweighted autoencoded variational Bayes for enhanced sampling (RAVE).” We study two molecular systems—urea and glycine—in explicit all-atom water, due to their enrichment in polymorphic structures and common utility in commercial applications. From our simulations, we observe multiple back-and-forth nucleation events of different polymorphs from homogeneous solution; from these trajectories, we calculate the relative ranking of finite-sized polymorph crystals embedded in solution, in terms of the free-energy difference between the finite-sized crystal polymorph and the original solution state. We further observe that the obtained reaction coordinates and transitions are highly nonclassical.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Nucleation mechanism of multiple-order parameter ferroelectric domain wall motion in hafnia

Ferroelectric hafnia exhibits promising robust polarization and silicon compatibility for ferroelectric devices. Unfortunately, it suffers from difficult polarization switching. Methods to enable easier polarization switching are needed, and the underlying reason for this switching difficulty is not understood. Here, we investigated the 180° domain walls of hafnia and their motion through nucleation. We found that the domains of multiple-order parameter hafnia possess complicated three-dimensional dipole patterns and lead to domain walls of different symmetry. The most common domain wall type is a complex domain wall involving reversal of both polarization and tetragonality order parameters. This domain wall symmetry ensures a good matching of the dipoles perpendicular to the domain wall, which leads to low domain wall energy. However, this ensures a sharp, high-energy, charged domain wall on the edges of nuclei that results in difficult nucleation. Thus, this domain wall is too stable to move, which explains the switching difficulty of hafnia. By contrast, another simple domain wall, involving only polarization reversal, has a poor matching of dipoles perpendicular to the domain wall. This leads to higher domain wall energy and ensures a diffusive and low-energy charged domain wall that enables easier nucleation. This simple domain wall is thus not too stable and easier to move. Our theory advances domain wall nucleation theory from the field of conventional single-order parameter to multiple-order parameters. We propose controlling the populations of different domain wall types in hafnia as a way to enable fast polarization switching and lower coercive fields.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Multistage nucleation pathway in LiF molten salt mirrors the crystal–melt interface structure

Despite over a century of studies, fundamental questions remain about the processes governing crystal nucleation from melts or solutions. Research over the past three decades has presented mounting evidence for kinetic pathways of crystal nucleation that are more complex than envisioned by the simplest forms of classical theory. Such observations have been presented for colloidal and elemental systems with covalent and metallic bonding. Despite the technological and geochemical importance of molten salts, similar studies for these ionically bonded systems are currently lacking. Here we develop a machine learning interatomic potential for a model ionic system: LiF. The potential features quantum-level accuracy for both liquid and multiple solid polymorphs over wide temperature and pressure ranges and accurately reproduces experimentally measured properties. Thanks to the efficiency of the potential, which enables microsecond-scale molecular dynamics simulations, induction times for nucleation of LiF solids from their melts are computed over a range of undercoolings. With the aid of a set of robust local order parameters established here, the simulations reveal that homogeneous crystal nucleation in undercooled melts preferentially initiates from liquid regions showing slow dynamics and high bond orientational order simultaneously, and the second-shell order of both precritical nuclei and the surface of postcritical nuclei is dominated by hexagonal close packing and body-centered cubic local structure, even though the nucleus core is dominated by face-centered cubic structure corresponding to the stable rocksalt crystal structure. Finally, we establish a connection between the crystallization pathway and the equilibrium crystal-melt interface structure.

Applied Physical Sciences↗
DOE OSTI2012

METHANE-NITROGEN BINARY NUCLEATION: A NEW MICROPHYSICAL MECHANISM FOR CLOUD FORMATION IN TITAN'S ATMOSPHERE

It is known that clouds are present in the troposphere of Titan; however, their formation mechanism, particle size, and chemical composition remain poorly understood. In this study, a two-component (CH{sub 4} and N{sub 2}) bin-microphysics model is developed and applied to simulate cloud formation in the troposphere of Titan. A new process, binary nucleation of particles from CH{sub 4} and N{sub 2} gases, is considered. The model is validated and calibrated by recent laboratory experiments that synthesize particle formation in Titan-like environments. Our model simulations show that cloud layers can be formed at about 20 km with a particle size ranging from one to several hundred {mu}m and number concentration 10{sup -2} to over 100 cm{sup -3} depending on the strength of the vertical updraft. The particles are formed by binary nucleation and grow via the condensation of both CH{sub 4} and N{sub 2} gases, with their N{sub 2} mole fraction varying from <10% in the nucleation stage to >30% in the condensation growth stage. The locally occurring CH{sub 4}-N{sub 2} binary nucleation mechanism is strong and could potentially be more important than the falling condensation nuclei mechanism assumed in many current models.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Modeling of Lithium Nucleation and Plating Kinetics Under Fast Charge Conditions

The onset of lithium nucleation and subsequent plating on the graphite particles is a challenging problem in the design of fast charging batteries. Here, a variational phase field formulation has been developed to initiate the nucleation of lithium particles based on the local plating overpotential conditions and allowing to predict the lithium plating under fast charge conditions. The model demonstrates that (1) at small charging current density, there is no nucleation and plating of metallic lithium, and no effect on the intercalation kinetics; (2) at intermediate charging current densities, initially a stagnated growth from isolated lithium nuclei is observed followed by a continuous growth of metallic lithium; (3) at large charging current densities, a continuous growth of metallic lithium resulting from coalescence of small nuclei into large nuclei decreases the excess interfacial energy, which in turn slows down the intercalation kinetics. The formulation sets the stage for predicting and evaluating the influence of various electrolyte compositions, graphite particle morphologies and electrode loadings on the nucleation and plating dynamics under fast charge conditions.

25 ENERGY STORAGE↗
DOE OSTI2022

Characterization and application of a high-resolution microfluidic device in atmospheric ice nucleation research and integrated science teaching

Ambient ice-nucleating particles (INPs) represent an important subset of aerosol particles that facilitate heterogeneous formation of ice crystals in the atmosphere, which can impact Earth system and energy. In this work, we developed an affordable high-resolution platform to replicate atmospheric immersion freezing through the unique capabilities of microfluidics to measure INP concentration of known ice nucleation active materials, as well as high-latitude soil samples. The new instrument produced comparable and extended freezing efficiency data for a multitude of samples over the temperature range of -5 to -35 °C as compared to an existing freezing assay within known uncertainties. Moreover, the new assay was integrated into science teaching at a primarily undergraduate and Hispanic-serving institute, contributing to fostering a deeper understanding of ice nucleation processes among college students, instilling their enthusiasm for science, and addressing the critical need for a well-informed citizenry. Student research assistants were involved in both research and pedagogical development processes. Three students from our team visited the Pacific Northwest National Laboratory to help characterize physicochemical properties of our test samples and to test modeling of atmospheric ice nucleation using a box model as well as a global climate model (E3SM) for the regional-scale conditions over the North Slope of Alaska (NSA) and Southern Great Plains (SGP). We also assessed student learning experience via hands-on training, research processes, and development of educational materials. On pre- and post-participation surveys and in exit interviews, students reported personal growth as advancements in breadth of experience, research-related skill sets, and regarding their educational and career goals. They also affirmed that the methods enacted incorporated the NASA Minority University Research and Education Program (MUREP) STEM Engagement Best Practices.

58 GEOSCIENCES↗
DOE OSTI2018

A Simple Technique to Improve Microcrystals Using Gel Exclusion of Nucleation Inducing Elements

A technique is described for generating large well diffracting crystals from conditions that yield microcrystals. Crystallization using this technique is both rapid (crystals appear in <1 h) and robust (48 out of 48 co-crystallized with a fragment library, compared with 26 out of 48 using conventional hanging drop). Agarose gel is used to exclude nucleation inducing elements from the remaining crystallization cocktail. The chemicals in the crystallization cocktail are partitioned into high concentration components (presumed to induce aggregation by reducing water activity) and low concentration nucleation agents (presumed to induce nucleation through direct interaction). The nucleation agents are then combined with 2% agarose gel and deposited on the crystallization shelf of a conventional vapor diffusion plate. The remaining components are mixed with the protein and placed in contact with the agarose drop. This technique yielded well diffracting crystals of lysozyme, cubic insulin, proteinase k, and ferritin (ferritin crystals diffracted to 1.43 Å). The crystals grew rapidly, reaching large size in less than one hour (maximum size was achieved in 1–12 h). This technique is not suitable for poorly expressing proteins because small protein volumes diffuse out of the agarose gel too quickly. Nonetheless, it is a useful technique for situations where crystals must grow rapidly (such as educational applications and preparation of beamline test specimens) and in situations where crystals must grow robustly (such as co-crystallization with a fragment library).

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1995

Containerless Liquid to Solid Nucleation Pathways in Two Representative Grades of Commercially Available Zirconium

Experimental measurements were conducted to determine the solid metal nucleation pathways of radiatively cooling, molten zirconium spheres of two different commercially available purity grades in a high-vacuum, high-temperature electrostatic levitator. The ensemble distribution of maximum undercooling temperatures was interpreted using Poisson statistics to determine the temperature dependence of the solid metal nucleation rate. For a sample of nominally 99.95% pure zirconium, the results are consistent with heterogeneous solid metal nucleation either on static catalyst particles at least ~30 nm diameter or on a surface coating. For a sample of nominally 99% pure zirconium, however, it appears that heterogeneous solid metal nucleation occurred either on a polydispersion of ~10 nm (mean diameter) static catalyst particles or on dynamic catalyst particles which precipitated from a solution which became supersaturated as the melt cooled. A quantitative analysis of the compositions of both samples suggests that the catalysts probably consisted of one or more of the following elements: niobium, molybdenum, hafnium, and oxygen.

containerless, nucleation, zirconium↗
DOE OSTI2020

Controlled Nucleation and Stabilization of Ferroelectric Domain Wall Patterns in Epitaxial (110) Bismuth Ferrite Heterostructures

Ferroelectric domain walls, topological entities separating domains of uniform polarization, are promising candidates as active elements for nanoscale memories. In such applications, controlled nucleation and stabilization of domain walls are critical. In this work, using in situ transmission electron microscopy and phase-field simulations, a controlled nucleation of vertically oriented 109° domain walls in (110)-oriented BiFeO 3 (BFO) thin films is reported. In the switching experiment, reversed domains that are nucleated preferentially at the nanoscale edges of the “crest and sag” pattern-like electrode under external bias subsequently grow into a stable stripe configuration. In addition, when triangular pockets (with an in-plane polarization component) are present, these domain walls are pinned to form stable flux-closure domains. Phase field simulations show that i) field enhancement at the edges of the electrode causes site-specific domain nucleation, and ii) the local electrostatics at the domain walls drives the formation of flux closure domains, thus stabilizing the striped pattern, irrespective of the initial configuration. The results demonstrate how flux closure pinning can be exploited in conjunction with electrode patterning and substrate orientation to achieve a desired topological defect configuration. These insights constitute critical advancements in exploiting domain walls in next generation ferroelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Heterogeneous Nucleating Agent for High‐Boiling‐Point Nonhalogenated Solvent‐Processed Organic Solar Cells and Modules

Abstract High‐boiling‐point nonhalogenated solvents are superior solvents to produce large‐area organic solar cells (OSCs) in industry because of their wide processing window and low toxicity; while, these solvents with slow evaporation kinetics will lead excessive aggregation of state‐of‐the‐art small molecule acceptors (e.g. L8‐BO), delivering serious efficiency losses. Here, a heterogeneous nucleating agent strategy is developed by grafting oligo (ethylene glycol) side‐chains on L8‐BO (BTO‐BO). The formation energy of the obtained BTO‐BO; while, changing from liquid in a solvent to a crystalline phase, is lower than that of L8‐BO irrespective of the solvent type. When BTO‐BO is added as the third component into the active layer (e.g. PM6:L8‐BO), it easily assembles to form numerous seed crystals, which serve as nucleation sites to trigger heterogeneous nucleation and increase nucleation density of L8‐BO through strong hydrogen bonding interactions even in high‐boiling‐point nonhalogenated solvents. Therefore, it can effectively suppress excessive aggregation during growth, achieving ideal phase‐separation active layer with small domain sizes and high crystallinity. The resultant toluene‐processed OSCs exhibit a record power conversion efficiency (PCE) of 19.42% (certificated 19.12%) with excellent operational stability. The strategy also has superior advantages in large‐scale devices, showing a 15.03‐cm 2 module with a record PCE of 16.35% (certificated 15.97%).

Chemistry↗
DOE OSTI2025

Nucleation rate controlled grain boundary and lattice creep

Nucleation versus diffusion rate-limited bicrystal and single crystal creep exhibit different scaling dependencies that enable the mechanisms to be isolated when measured as a function of sample size. It has recently been suggested that nucleation rate-limited kinetic models generally describe the non-Newtonian portion of the creep response well, but more direct evidence is required. This work analyzes the grain boundary creep response of UO 2 , a pyrochlore high entropy oxide, silver, and palladium, along with the lattice creep of silver using small-scale in situ loading in the transmission electron microscope. At small sizes, each system exhibits scale dependence associated with nucleation rate-limited kinetics. Fits of the data produce activation volumes on the order of a few Burgers vectors cubed with positive temperature coefficients as expected for nucleation kinetics. The activation enthalpies fall in the range of about 0.4 eV to 1.7 eV, being lower for the metals and higher for the oxides.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Automated processing of environmental transmission electron microscopy images for quantification of thin film dewetting and carbon nanotube nucleation dynamics

We report scalable production of carbon nanotubes (CNTs) requires catalysts and reaction conditions that provide high nucleation efficiency. In situ characterization methods such as environmental transmission electron microscopy (ETEM) can reveal fundamental mechanisms of synthesis, but to date have primarily provided qualitative observations on small sample sizes. Here, quantitative analysis is performed using high-resolution, high-rate video capture of ETEM experimentation coupled with automated image processing, involving computer vision algorithms and convolutional neural networks. By this approach, we detect distinct nanoparticle formation from an alumina-supported iron thin film and subsequent CNT nucleation from the nanoparticles. The statistical summary of particles in each video shows that, compared to a H 2 -only atmosphere, pretreatment of the catalyst with carbon added to the H 2 atmosphere results in a smaller average particle diameter, a 2-fold increase in particle density (to 5300 particles/μm 2 ), a 3-fold increase in CNT nucleation efficiency (to 92%), and more than a 5-fold increase in CNT density (to 4800/μm 2 ). Addition of carbon during exposure to H 2 is also more effective than NH 3 at dewetting the catalyst film and increasing the CNT nucleation efficiency, in spite of NH 3 being a stronger reducing agent for iron. Insights from this study are applicable to improving CNT yield and productivity in both batch-style and continuous processes.

25 ENERGY STORAGE↗