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Results for “heterogeneous nucleation”

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 OSTI2022

A facile approach for site-selective and large-area growth of MoS 2 through heterogeneous nucleation

Heterogeneous nucleation could be an effective approach to producing an array of transition metal dichalco-genides (TMDs) at controlled locations on a substrate. In this study, we prepared Pt mesa structures on the substrate to induce heterogeneous nucleation of MoS 2 during chemical vapor deposition (CVD) and investigated the adsorption of nuclei using Monte Carlo (MC) simulations. The MC simulations suggest that the site-selectivity of MoS 2 dramatically drops when the CVD growth time goes beyond the critical time at which nuclei fully cover the Pt mesas, and such critical time can be delayed when the size of Pt mesas increases. Our experimental observations on a clean array of MoS 2 successfully synthesized on 10 um-width square Pt mesas but not on 4 um -width square Pt mesas support the MC simulation. We further designed a simple method employing dummy substrates to increase the yield of the site-selective MoS 2 array. Computational fluid dynamics (CFD) simulation reveals that such dummy substrates restrict the precursor concentration and provide a confined channel for the precursors to react slowly, which benefits producing large-area and site-selective MoS 2 . Furthermore, compared with conventional CVD, the total coverage of site-selective MoS 2 has enlarged by seven times using dummy substrates.

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

Three Distinctive Steps for Heterogeneous Nucleation of Tunnel-Structured Mn Oxide on Quartz under Light Exposure

Natural manganese (Mn) oxide coatings, resulting from the heterogeneous nucleation on foreign substances, have garnered interest based on their importance in the reaction with organic substances and in environmental systems. However, the heterogeneous nucleation of the natural Mn oxide coatings still remains elusive. Here, via fast photochemical oxidation of Mn 2+ (aq), we show that Mn(IV) oxide nuclei form and aggregate on quartz in three distinct successive stages: (i) a nanocrystalline film of unaligned grain forms, (ii) nanoislands develop on the film, and (iii) nanorods form on the nanoislands. Each stage has different crystalline structures and forms by aligned attachment of nanoscale precursors on the preceding surface. Crystal lattice analyses confirm the crystalline development, from the short-range order of the Mn oxide film to the long-range order of the nanorods. Also, the heterogeneous nucleation observed in this work produced groutellite-like tunnel structures of Mn oxide on quartz. Furthermore, this revealed pathway of the heterogeneous nucleation can offer a new perspective on the variety of poorly crystalline structures of natural Mn oxides found in the environment, which can affect elemental redox cycles, contaminant sequestration and removal, and soil carbon storage.

Aligned attachment↗
DOE OSTI2025

How are Heterogeneous Nucleation Rate Observations Influenced by Instrument Resolution?

Experimental measurements of the heterogeneous nucleation rate rely on counting the number of nuclei with time. However, the size of a thermodynamically stable nucleus is often a few nanometers in diameter and is below the resolution of most (in situ) measurement techniques that provide a statistically valid sample. Due to the finite resolution of the instruments and analysis methods, it is challenging to capture the incipient nuclei and the subsequent evolution of nuclei density over time. In this work, we demonstrate the impact of instrument resolution on observed nuclei densities by comparing numerical modeling with experimental results. Further, to achieve this, we implemented heterogeneous nucleation within the pore-scale reactive transport modeling framework using classical nucleation theory (CNT). We compared the modeling results with nucleation rates measured using X-ray nanotomography (XnT) and evaluated how these impact the apparent values of the prefactor and interfacial energy based on CNT and the crystal growth rate. Specifically, we applied a resolution threshold (artificial resolution limit) in the model during nuclei counting to resemble an experimental resolution, ranging from 15 to 500 nm. The findings reveal that the instrument resolution significantly impacts the apparent prefactor and interfacial energy. Both apparent prefactor and interfacial energy decrease with a decrease in the instrument resolution. While deviation in the prefactor due to resolution is anticipated, those in the interfacial energy are unexpected. The approach described here allows one to correct apparent nucleation rates that depend on the instrument’s resolution to derive “intrinsic” CNT parameters for the prefactor and interfacial energy.

47 OTHER INSTRUMENTATION↗
NASA NTRS1991

Scaling properties of induction times in heterogeneous nucleation

The heterogeneous-to-homogeneous induction time ratio is obtained as a function of the contact angle in the asymptotic limit of a high nucleation barrier. Model-dependent corrections to t(ind) are investigated, particularly in cases of the Turnbull-Fisher model used in numerical simulations by Greer et al. (1990).

Shneidman, Vitaly A.↗
NASA NTRS1971

Heterogeneous nucleation of gamma prime in Al-Ag and Al-Ag /Cd or Cu/ alloys.

Results of transmission electron microscopy studies of heterogeneous nucleation of the metastable gamma prime phase were made in binary and ternary alloys of Al-5 at. % Ag, Al-4.8 at. % Ag-0.15 at. % Cd, and Al-4.8 at. % Ag-0.2 at. % Cu. Heterogeneous nucleation of gamma prime was found to be associated with four types of dislocations, regardless of the quenching treatment or alloy additions which were used. Nucleation was found to occur on: (a) jogged dislocations; (b) helical dislocations; (c) dislocation loops; (d) heterogeneous climb sources. Only one nucleation mechanism was found to be unique to the ternary alloys: that of nucleation on heterogeneous climb sources.

Passoja, D. E.↗
DOE OSTI2025

Impact of Interfacial Structure on Heterogeneous Nucleation of Amorphous Carbonates

For this work, classical molecular dynamics simulations were performed to provide physical insight into the impact of interfacial structure on the heterogeneous nucleation of amorphous calcium carbonate (ACC, CaCO 3 ·H 2 O) and amorphous magnesium carbonate (AMC, MgCO 3 ·H 2 O) by using α-quartz as a model substrate. Interfacial structure and energies were computed for ACC and AMC in contact with the (100), (001), and (101) α-quartz surfaces. The simulations showed α-quartz surfaces drew water molecules out of the carbonate nuclei to form a partial hydration layer. The formation of a partial hydration layer and its disruption to the ACC/AMC structure meant the α-quartz–ACC/AMC interfaces were not energetically favored relative to separate α-quartz–water and ACC/AMC–water interfaces and, thus, homogeneous ACC/AMC nucleation was favored over heterogeneous nucleation. The CMD simulations hence provided an atomic-level explanation for a reported nonclassical growth mechanism whereby carbonate minerals grow via homogeneous nucleation and subsequent surface attachment of amorphous intermediates.

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

Surface Functional Groups Affect Iron (Hydr)oxide Heterogeneous Nucleation: Implications for Membrane Scaling

Because of its favorable thermodynamics and fast kinetics, heterogeneous solid nucleation on membranes triggers early-stage mineral scaling. Iron (hydr)oxide, a typical membrane scale, initially forms as nanoparticles that interact with surface functional groups on membranes, but these nanoscale phenomena are difficult to observe in real time. In this study, we utilized in situ grazing incidence small angle X-ray scattering and ex situ atomic force microscopy to examine the heterogeneous nucleation of iron (hydr)oxide on surface functional groups commonly used in membranes, including hydroxyl (OH), carboxyl (COOH), and fluoro (F) groups. We found that, compared to nucleation on hydrophilic OH- and COOH-surfaces, the high hydrophobicity of an F-modified surface significantly reduced the extents of both heterogeneously and homogeneously formed iron (hydr)oxide nucleation. Moreover, on the OH-surface, the high functional group density of 0.76 nmol/cm 2 caused faster heterogeneous nucleation than that on a COOH-surface, with a density of 0.28 ± 0.04 nmol/cm 2 . The F-surface also had the highest heterogeneous nucleation energy barrier (26 ± 0.6 kJ/mol), followed by COOH- (23 ±0.8 kJ/mol) and OH- (20 ± 0.9 kJ/mol) surfaces. The kinetic and thermodynamic information provided here will help us better predict the rates and extents of early-stage scaling of iron (hydr)oxide nanoparticles in membrane processes. Finally, this work provides both kinetic and thermodynamic information about iron (hydr)oxide nucleation controlled by membrane-related functional groups (OH, COOH, and F).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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↗
NASA NTRS1992

The influence of finite impurity size on heterogeneous nucleation

The effects of the finite size of impurities upon the heterogeneous nucleation rate is examined. Simple arguments based upon probability theory are used to find the relative nucleation rate, p(j), on particles containing j nuclei. The expression for p(j) is used in turn to compute the overall nucleation rate and average number of nuclei on an impurity as a function of time.

Weinberg, Michael C.↗
DOE OSTI2024

Effect of Nucleation Heterogeneity on Mineral Precipitation in Confined Environments

Abstract The formation of new mineral phases in confined environments, especially in porous media, is crucial for various geological processes like mineralization and diagenesis. The nucleation and precipitation of minerals are initiated at the microscale through fluid‐rock interaction, where dissolution of primary phases leads to supersaturated conditions and nucleation and growth of secondary ones. Previous research has focused primarily on either precipitation or nucleation, without fully exploring their combined impact. Our study introduces a computational framework that integrates classical nucleation theory with the micro‐continuum method. We validated our model by comparing with experiments, and discovered that different surface nucleation rate changes the mode of precipitation from a preferential to uniform precipitate textures. Furthermore, our study uncovered that the conventional deterministic precipitation method tends to underestimate the permeability of the porous matrix. In contrast, the new framework significantly improves model accuracy by incorporating preferential precipitation and heterogeneous nucleation.

58 GEOSCIENCES↗
DOE OSTI2024

Mechanisms of electromagnetic field control on mineral scaling in brackish water reverse osmosis: Combined homogenous and heterogeneous nucleation

Electromagnetic field (EMF) treatment has emerged as a promising approach for scaling control due to its cost-effectiveness, simplicity, and low energy consumption. However, there is a limited understanding of the mechanisms by which applied EMF impacts mineral scaling in reverse osmosis (RO) systems. This has led to inconclusive and varied results and uncertainties regarding its effectiveness. This study elucidates the impacts of EMF on homogenous and heterogeneous nucleation and membrane performance during RO desalination of different feedwaters. Our results reveal that EMF exhibits greater efficacy in treating near-saturated water (SI∼0), especially when coupled with extended hydraulic flushing (HF). For saturated brackish water desalination, heterogeneous scaling predominantly occurs on membrane surfaces, with the effectiveness of EMF in inhibiting scaling primarily attributed to the hydration effect. In supersaturated solutions, EMF promotes bulk precipitation due to the magnetohydrodynamic effect, quickly blocking membrane pores. Thus, when the saturation reaches a certain high level during RO desalination, magnetohydrodynamic EMF effects can accelerate flux decline caused by homogeneous scaling. In conclusion, this work provides an efficient method for predicting EMF efficiency, emphasizing the importance of saturation conditions and HF cleaning duration in determining membrane performance, suggesting these show promise for improving undersaturated or near-saturated feedwater desalination via RO.

42 ENGINEERING↗
DOE OSTI2021

Opposing Effects of Impurity Ion Sr 2+ on the Heterogeneous Nucleation and Growth of Barite (BaSO 4 )

Nucleation of barite (BaSO 4 ) has broad implications in geological, environmental, and materials sciences. While impurity metals are common, our understanding of how they impact nucleation remains dim. In this work, we used classical optical microscopy compared to fast X-ray nanotomography (XnT) to investigate heterogeneous nucleation of barite on silica in situ with Sr 2+ as an impurity ion. The observed barite nucleation rates were consistent with classical nucleation theory (CNT), where barite crystals displayed a nonuniform size distribution, exhibiting distinct morphologies and incubation periods in Sr-free solutions. While undetectable with optical microscopy, nanotomography revealed that addition of Sr2+ enhances nucleation rates driven by the pre-factor in CNT, likely because both adsorbed Ba 2+ and Sr 2+ act as precursor sites on which nucleation occurs. Sr 2+ simultaneously inhibits growth, however, leading to a homogeneous distribution of smaller crystals. This finding will enable an improved predictive understanding of nucleation in natural and synthetic environments.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A new parameterization of ice heterogeneous nucleation coupled to aerosol chemistry in WRF-Chem model version 3.5.1: evaluation through ISDAC measurements

In the Arctic, during polar night and early spring, ice clouds are separated into two leading types of ice clouds (TICs): (1) TIC1 clouds characterized by a large concentration of very small crystals and TIC2 clouds characterized by a low concentration of large ice crystals. Using a suitable parameterization of heterogeneous ice nucleation is essential for properly representing ice clouds in meteorological and climate models and subsequently understanding their interactions with aerosols and radiation. Here, we describe a new parameterization for ice crystal formation by heterogeneous nucleation in water-subsaturated conditions coupled to aerosol chemistry in the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). The parameterization is implemented in the Milbrandt and Yau (2005a, b) two-moment cloud microphysics scheme, and we assess how the WRF-Chem model responds to the run-time interaction between chemistry and the new parameterization. Well-documented reference cases provided us with in situ data from the spring 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) over Alaska. Our analysis reveals that the new parameterization clearly improves the representation of the ice water content (IWC) in polluted or unpolluted air masses and shows the poor performance of the reference parameterization in representing ice clouds with low IWC. The new parameterization is able to represent TIC1 and TIC2 microphysical characteristics at the top of the clouds, where heterogenous ice nucleation is most likely occurring, even with the known bias of simulated aerosols by WRF-Chem over the Arctic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Interpreting experimental measurements of helium bubbles using stochastic cluster dynamics models of heterogeneous nucleation and growth in irradiated ferritic alloys

Among a number of other advantageous features, ferritic/martensitic steels are being considered as fusion reactor structural materials due to their low intrinsic swelling under irradiation. However, under high-energy neutron irradiation, He produced through (n, α) reactions stabilizes vacancy clusters, which then act as seeds for bubble formation and growth, negating the intrinsic swelling resistance of these alloys. Standard models of irradiation damage accumulation and microstructural evolution consider homogeneous nucleation as the basis for bubble formation and growth. However, this generally does not explain the large bubble densities and sizes observed experimentally under a number of different conditions. Here, we propose a more realistic physical model of bubble nucleation, formation, and growth designed to capture recent experimental measurements of He-bubble formation and evolution during co-implantation of He and Fe ions in model ferritic alloys. We find that experimental results are explained only when the following three features are considered simultaneously: (i) heterogeneous nucleation of He-vacancy bubbles at defect sinks (e.g., dislocations, grain boundaries, and second-phase precipitates), (ii) nucleation and growth of bubbles via the ‘trap mutation’ mechanism (i.e., spontaneous production of Frenkel pairs due to absorption of He atoms), and (iii) transition from a growth-limited, He-stabilized bubble regime to a ‘runaway’ void-type growth scenario. The model is implemented into a stochastic cluster dynamics framework that takes advantage of cluster size grouping methods to accelerate the simulations, allowing us to reach 10 dpa of simulated irradiated dose, and to capture cluster sizes in excess of 20 nm. Further, a careful extrapolation exercise conducted assuming classical nucleation theory leads to excellent agreement with the experimental measurements at 50 dpa of irradiation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ion correlations drive charge overscreening and heterogeneous nucleation at solid–aqueous electrolyte interfaces

Significance Ion distributions at charged solid–water interfaces, referred to as the electrical double layer (EDL), are poorly understood at high ion concentrations, in part due to the lack of molecular-scale descriptions of the interactions between adsorbed hydrated ions. Here, direct visualization of the salinity-dependent evolution of EDL structure reveals molecular origins of nonclassical transformation of the EDL, in which charge overscreening and heterogeneous nucleation are driven by ion–ion correlations at the interfaces. This manifestation of the atomistic basis of nonclassical behaviors provides a much-needed understanding of the impact of ion cooperativity at charged interfaces for the development of predictive models for element transport in natural environments and advanced technologies for material growth and synthesis in saline environments.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Localized Heterogeneous Nucleation for Vapor‐Assisted Sequential Deposition of Metal Halide Perovskites

Vapor-assisted hybrid two-step deposition, which combines thermally evaporated inorganic layers with solution-processed organic halides to form halide perovskites, has emerged as a scalable and industry-compatible route for textured tandem photovoltaics. However, this process is often hindered by reaction-limited phase formation, particularly when compact, non-porous, and highly crystalline inorganic layers formed by thermal evaporation restrict subsequent conversion, resulting in incomplete reaction and pronounced depth-dependent heterogeneity. In this study, we introduce a strategy to regulate the inorganic precursor layer by incorporating localized heterogeneous nucleation sites. Sparsely distributed hydrophilic metal oxide species serve as effective nucleation centers during vapor deposition, enabling effective control over film morphology and crystal orientation from the early stages of growth. This tailored inorganic framework facilitates the subsequent incorporation of organic halides, alleviating reaction limitations and suppressing residual unreacted precursors. Consequently, the perovskite films exhibit improved stoichiometric uniformity and enhanced optoelectronic quality, enabling wide-bandgap perovskite solar cells with markedly improved performance and operational stability. This work provides important mechanistic insight into crystal growth engineering of vapor-deposited perovskite thin films.

nucleation↗
NASA NTRS1992

A case of type I polar stratospheric cloud formation by heterogeneous nucleation

The NASA ER-2 aircraft flew on January 24, 1989, from Stavanger to Spitsbergen, Norway, at the 430-440 K potential temperature surface (19.2-19.8 km pressure altitude). Aerosols were sampled continuously by an optical particle counter (PMS-FSSP300) for concentration and size analyses, and during five 10-min intervals by four wire and one replicator impactor for concentration, size, composition, and phase analysis. During sampling, the air saturation of H2O with respect to ice changed from 20 to 100 percent, and of HNO3 with respect to nitric acid trihydrate (NAT) from subsaturation to supersaturation. Data from both instruments indicate a condensation of hydrochloric acid and, later, nitric acid on the background aerosol particles as the ambient temperature decreases along the flight track. This heterogeneous nucleation mechanism generates type I polar stratospheric cloud particles of 10-fold enhanced optical depth, which could play a role in stratospheric ozone depletion.

Pueschel, R. F.↗