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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 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Nonlinear bubble nucleation and growth following filament and white-light continuum generation induced by a single-shot femtosecond laser pulse into dielectrics based on consideration of the time scale

Bubble nucleation and growth following plasma channeling (filament) and white-light continuum in liquid irradiated by a single-shot fs-pulse were experimentally investigated with close observation of the time scale. Making full use of a new confocal system and time-resolved visualization techniques, we obtained evidence suggestive of a major/minor role of the non-linear/thermal effects during the fs-pulse-induced bubble's fountainhead (10{sup −13} s) and growth (10{sup −7} s), which was never observed with the use of the ns-pulse (i.e., optic cavitation). In this context, the fs-pulse-induced bubble is not an ordinary optic cavitation but rather is nonlinear-optic cavitation. We present the intrinsic differences in the dominant-time domain of the fs-pulse and ns-pulse excitation, and intriguingly, a mere hundred femtoseconds' excitation predetermines the size of the bubble appearing several microseconds after irradiation. That is, the nucleation happens temporally beyond a six-order-of-magnitude difference.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Direct observation of atomic-level nucleation and growth processes from an ultrathin metallic glass films

Till date, there have been no direct atomic-level experimental observations of the earliest stages of the nucleation and growth processes of nanocrystals formed by thermally induced crystallization in ultrathin metallic glasses (MGs). Here, we present a study of the crystallization process in atomically thin and highly stable MG films using double spherical aberration-corrected scanning transmission electron microscopy (Cs-TEM). Taking advantage of the stability of MG films with a slow crystallization process and the atomic-level high resolution of Cs-TEM, we observe the formation of the nucleus precursor of nanocrystals formed by atom aggregation followed by concomitant coalescence and stepwise evolution of the shape of the nanocrystals with a monodispersed and separated bimodal size distribution. Molecular dynamics simulation of the atomic motion in the glass film on a rigid amorphous substrate confirms the stepwise evolution processes of atom aggregation, cluster formation, cluster movement on the substrate, and cluster coalescence into larger crystalline particles. Our results might provide a better fundamental understanding of the nucleation and growth processes of nanocrystals in thin MG films.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

First passage times in homogeneous nucleation: Dependence on the total number of particles

Motivated by nucleation and molecular aggregation in physical, chemical, and biological settings, we present an extension to a thorough analysis of the stochastic self-assembly of a fixed number of identical particles in a finite volume. We study the statistics of times required for maximal clusters to be completed, starting from a pure-monomeric particle configuration. For finite volumes, we extend previous analytical approaches to the case of arbitrary size-dependent aggregation and fragmentation kinetic rates. For larger volumes, we develop a scaling framework to study the first assembly time behavior as a function of the total quantity of particles. We find that the mean time to first completion of a maximum-sized cluster may have a surprisingly weak dependence on the total number of particles. We highlight how higher statistics (variance, distribution) of the first passage time may nevertheless help to infer key parameters, such as the size of the maximum cluster. Finally, we present a framework to quantify formation of macroscopic sized clusters, which are (asymptotically) very unlikely and occur as a large deviation phenomenon from the mean-field limit. We argue that this framework is suitable to describe phase transition phenomena, as inherent infrequent stochastic processes, in contrast to classical nucleation theory.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Evidence for a liquid-liquid critical point in supercooled water within the E3B3 model and a possible interpretation of the kink in the homogeneous nucleation line

Supercooled water exhibits many thermodynamic anomalies, and several scenarios have been proposed to interpret them, among which the liquid-liquid critical point (LLCP) hypothesis is the most commonly discussed. We investigated Widom lines and the LLCP of deeply supercooled water, by using molecular dynamics simulation with a newly reparameterized water model that explicitly includes three-body interactions. Seven isobars are studied from ambient pressure to 2.5 kbar, and Widom lines are identified by calculating maxima in the coefficient of thermal expansion and the isothermal compressibility (both with respect to temperature). From these data we estimate that the LLCP of the new water model is at 180 K and 2.1 kbar. The oxygen radial distribution function is calculated along the 2 kbar isobar. It shows a steep change in the height of its second peak between 180 and 185 K, which indicates a transition between the high-density liquid and low-density liquid phases and which is consistent with the ascribed location of the critical point. The good agreement of the height of the second peak of the radial distribution function between simulation and experiment at 1 bar, as a function of temperature, supports the validity of the model. The location of the LLCP within the model is close to the kink in the experimental homogeneous nucleation line. We use existing experimental data to argue that the experimental LLCP is at 168 K and 1.95 kbar and speculate how this LLCP and its Widom line might be responsible for the kink in the homogeneous nucleation line.

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

Observation of propane cluster size distributions during nucleation and growth in a Laval expansion

We report on molecular-level studies of the condensation of propane gas and propane/ethane gas mixtures in the uniform (constant pressure and temperature) postnozzle flow of Laval expansions using soft single-photon ionization by vacuum ultraviolet light and mass spectrometric detection. The whole process, from the nucleation to the growth to molecular aggregates of sizes of several nanometers (∼5 nm), can be monitored at the molecular level with high time-resolution (∼3 μs) for a broad range of pressures and temperatures. For each time, pressure, and temperature, a whole mass spectrum is recorded, which allows one to determine the critical cluster size range for nucleation as well as the kinetics and mechanisms of cluster-size specific growth. The detailed information about the size, composition, and population of individual molecular clusters upon condensation provides unique experimental data for comparison with future molecular-level simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Nucleation and stabilization of carbon-rich structures in interstellar media

We study the conditions under which carbon clusters of different sizes form and stabilize. We describe the approach to equilibrium by simulating tenuous carbon gas dynamics to long times. First, we use reactive molecular dynamics simulations to describe the nucleation of long chains, large clusters, and complex cage structures in carbon- and hydrogen-rich interstellar gas phases. We study how temperature, particle density, the presence of hydrogen, and carbon inflow affect the nucleation of molecular moieties with different characteristics, in accordance with astrophysical conditions. We extend the simulations to densities that are orders of magnitude lower than current laboratory densities, to temperatures that are relevant to circumstellar environments of planetary nebulae, and microsecond formation times. We correlate cluster size distributions from the simulations with thermodynamic equilibrium at low temperatures and gas densities, where entropy plays a significant role.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Nucleation and growth process of atomic layer deposition platinum nanoparticles on strontium titanate nanocuboids

Uniform, well-dispersed platinum nanoparticles were grown on SrTiO 3 nanocuboids via atomic layer deposition (ALD) using (methylcyclopentadienyl)trimethylplatinum (MeCpPt(Me)3) and water. For the first half-cycle of the deposition particles formed through two sequential processes: initial nucleation and growth. The final particle size after a single complete ALD cycle was dependent on the reaction temperature which alters the net Pt deposition per cycle. Additional cycles resulted in further growth of previously formed particles. However, the increase in size per cycle during additional ALD cycles, beyond the first, was significantly lower as less Pt was deposited due to carbonaceous material that partially covers the surface and prevents further MeCpPt(Me) 3 adsorption and reaction. The increase in particle size was also temperature dependent due to changes in the net Pt deposition. Pt nanoparticles increased in size by 59% and 76% after 15 ALD cycles for reaction temperatures of 200 °C and 300 °C, respectively. There was minimal change in the number of particles per unit area as a function of reaction time, indicating that there was minimal Ostwald ripening or secondary nucleation for the reaction conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Synthetic magnetohydrodynamics in Bose-Einstein condensates and routes to vortex nucleation

Engineering of synthetic magnetic flux in Bose-Einstein condensates [Lin et al., Nature (London) 462, 628 (2009)] has prospects for attaining the high vortex densities necessary to emulate the fractional quantum Hall effect. We analytically establish the hydrodynamical behavior of a condensate in a uniform synthetic magnetic field, including its density and velocity profile. Importantly, we find that the onset of vortex nucleation observed experimentally corresponds to a dynamical instability in the hydrodynamical solutions and reveal other routes to instability and anticipated vortex nucleation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Convenient analytical formula for cluster mean diameter and diameter dispersion after nucleation burst

Here, we propose an alternative method of estimating the mean diameter and dispersion of clusters of particles, formed in a cooling gas, right after the nucleation stage. Using a moment model developed by Friedlander [S. K. Friedlander, Ann. N. Y. Acad. Sci. 404, 354 (1983)], we derive an analytic relationship for both cluster mean diameter and diameter dispersion as a function of two of the characteristic times of the system: the cooling time and the primary constituents collision time. These formulas can be used to predict diameter and dispersion variation with process parameters, such as the initial primary constituents' concentration or cooling rate. It is also possible to use them as an input to the coagulation stage, without the need to compute complex cluster generation during the nucleation burst. We compared our results with a nodal code (NGDE) and got excellent agreement.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Size-Dependent Nucleation in Crystal Phase Transition from Machine Learning Metadynamics

In this Letter, we present a framework that combines machine learning potential (MLP) and metadynamics to investigate solid-solid phase transition. Here, based on the spectral descriptors and neural networks regression, we develop a scalable MLP model to warrant an accurate interpolation of the energy surface where two phases coexist. Applying it to the simulation of B4–B1 phase transition of GaN under 50 GPa with different model sizes, we observe sequential change of the phase transition mechanism from collective modes to nucleation and growths. When the size is at or below 128 000 atoms, the nucleation and growth appear to follow a preferred direction. At larger sizes, the nuclei occur at multiple sites simultaneously and grow to microstructures by passing the critical size. The observed change of the atomistic mechanism manifests the importance of statistical sampling with large system size in phase transition modeling.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Domain nucleation across the metal-insulator transition of self-strained V 2 O 3 films

Bulk V 2 O 3 features concomitant metal-insulator (MIT) and structural (SPT) phase transitions at T C ~ 160 K. In thin films, where the substrate clamping can impose geometrical restrictions on the SPT, the epitaxial relation between the V 2 O 3 film and substrate can have a profound effect on the MIT. Here we present a detailed characterization of domain nucleation and growth across the MIT in (001)-oriented V 2 O 3 films grown on sapphire. By combining scanning electron transmission microscopy (STEM) and photoelectron emission microscopy (PEEM), we imaged the MIT with planar and vertical resolution. We observed that upon cooling, insulating domains nucleate at the top of the film, where strain is lowest, and expand downwards and laterally. This growth is arrested at a critical thickness of 50 nm from the substrate interface, leaving a persistent bottom metallic layer. As a result, the MIT cannot take place in the interior of films below this critical thickness. However, PEEM measurements revealed that insulating domains can still form on a very thin superficial layer at the top interface. Our results demonstrate the intricate spatial complexity of the MIT in clamped V 2 O 3 , especially the strain-induced large variations along the c axis. Finally, engineering the thickness-dependent MIT can provide an unconventional way to build out-of-plane geometry devices by using the persistent bottom metal layer as a native electrode.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Simulation of nucleation and growth of atomic layer deposition phosphorus for doping of advanced FinFETs

Simulations for the nucleation and growth of phosphorus films were carried out using density functional theory. The surface was represented by a Si{sub 9}H{sub 12} truncated cluster surface model with 2 × 1-reconstructured (100) Si-OH terminations for the initial reaction sites. Chemistries included phosphorous halides (PF{sub 3}, PCl{sub 3}, and PBr{sub 3}) and disilane (Si{sub 2}H{sub 6}). Atomic layer deposition (ALD) reaction sequences were illustrated with three-dimensional molecular models using sequential PF{sub 3} and Si{sub 2}H{sub 6} reactions and featuring SiFH{sub 3} as a byproduct. Exothermic reaction pathways were developed for both nucleation and growth for a Si-OH surface. Energetically favorable reactions for the deposition of four phosphorus atoms including lateral P–P bonding were simulated. This paper suggests energetically favorable thermodynamic reactions for the growth of elemental phosphorus on (100) silicon. Phosphorus layers made by ALD are an option for doping advanced fin field-effect transistors (FinFETs). Phosphorus may be thermally diffused into the silicon or recoil knocked in; simulations of the recoil profile of phosphorus into a FinFET surface are illustrated.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Precursor dependent nucleation and growth of ruthenium films during chemical vapor deposition

Nucleation and film growth characteristics are reported during chemical vapor deposition of Ru on SiO{sub 2} using triruthenium dodecacarbonyl [Ru{sub 3}(CO){sub 12}] and ruthenium bis(di-t-butylacetamidinate) dicarbonyl [Ru({sup t}Bu-Me-amd){sub 2}(CO){sub 2}]. Films grown from Ru{sub 3}(CO){sub 12} follow the three dimensional (3D) Volmer–Weber growth mode. In contrast, films grown from Ru({sup t}Bu-Me-amd){sub 2}(CO){sub 2} follow the pseudo-layer-by-layer growth mode with two dimensional wetting layer islands forming before 3D particle growth is observed on the islands. A relationship between free isolated hydroxyl [(Si-OH){sub i}] group density and Ru nucleation density is found for Ru{sub 3}(CO){sub 12} and is associated with (Si-OH){sub i} acting as the reaction sites for activation of Ru{sub 3}(CO){sub 12} and in turn generating an adjustable adatom concentration. Carbon monoxide and ammonia addition to the gas phase during film growth from Ru({sup t}Bu-Me-amd){sub 2}(CO){sub 2} lead to smoother films by inducing surface reconstructions during the 3D phase of pseudo-layer-by-layer growth; these gases also lead to films with lower resistivity and lower crystalline character.

42 ENGINEERING↗
DOE OSTI2016

MD simulation of plastic deformation nucleation in stressed crystallites under irradiation

The investigation of plastic deformation nucleation in metals and alloys under irradiation and mechanical loading is one of the topical issues of materials science. Specific features of nucleation and evolution of the defect system in stressed and irradiated iron, vanadium, and copper crystallites were studied by molecular dynamics simulation. Mechanical loading was performed in such a way that the modeled crystallite volume remained unchanged. The energy of the primary knock-on atom initiating a cascade of atomic displacements in a stressed crystallite was varied from 0.05 to 50 keV. It was found that atomic displacement cascades might cause global structural transformations in a region far larger than the radiation-damaged area. These changes are similar to the ones occurring in the process of mechanical loading of samples. They are implemented by twinning (in iron and vanadium) or through the formation of partial dislocation loops (in copper).

36 MATERIALS SCIENCE↗
DOE OSTI2017

Possible Mechanism for Formation of Nonwettable “Dry Spots” on a Heated Surface during Nucleate Pool Boiling: II. Feedwater Stop Regime

The problems of simulation of heterogeneous nucleate pool boiling on a horizontal surface on the ascending branch of the boiling curve from the formation of a steam lens (SL) to the boiling crisis are considered. The proposed hypothesis provides in a number of cases a logically consistent interpretation of experiments and outlines the organizational principle of transferring the wall–liquid–steam system into the regime of nonwettable “dry spot” formation. The model includes the following types of nucleate boiling: (a) cyclic boiling with the contact line reverse to the bubble bottom center and bubble departure from the surface (at low heat flux q and the contact angle θ < 90°); (b) single steam bubble conversion into a steam lens, i.e., local film boiling with the possibility of spreading of a single “dry spot” at the variation of the contact angle θ ≥ 90°, and substantial growth of the departure diameter D{sub d} and SL lifetime τd; (c) formation of a single steam cluster of four SLs at a given pressure, the liquid underheating, and the average wall overheating.

42 ENGINEERING↗
DOE OSTI2017

Nucleation of Pre-precipitates in Structural Materials under Cascade-Forming Irradiation

A model is proposed to calculate pre-precipitate nucleation rate in supersaturated solid solutions under cascade-forming irradiation. Estimates of the rate of nucleation of copper-enriched clusters in Fe–Cu solid solutions with a copper concentration of 0.05–0.18 at. % due to reactor irradiation are carried out. A comparison with the experimental data on irradiation of structural materials shows that the formation of precipitate nuclei takes place in the cascade region involved at the final stages of cascade relaxation, whose volume is about two times higher than the cascade volume at the dynamic stage.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Estimation of Evaporation Rate from Gold-Silicon Alloy Based on the Nucleation Time and Nanowire Length Distributions

Abstract—: Nanowires are one of the most promising building blocks for various nanoelectronic devices. Nanowires are usually grown via the so-called vapor-liquid-solid mechanism on the surfaces activated by the droplets of a catalyst (e.g., Au). Here we theoretically studied the impact of the evaporation from the droplet on the nucleation statistics. Within the semi-analyticalapproach, we obtain the relation between the nucleation time distributions and the evaporation rate of atoms from the droplet. We analyze the Si NW length-time dependences to estimate theeffective lifetime of a silicon atom in a gold-silicon alloy at 550°C is about 5 s.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

Electromigration Effect on Vacancy Islands Nucleation on Si(100) Surface during Sublimation

By means of in situ ultrahigh vacuum reflection electron microscopy, the nucleation of vacancy islands on wide terraces of the Si(100) surface is investigated. The temperature dependence of the displacement of a vacancy island nucleation center is determined in the process of heating a sample with a dc electric current. On the basis of a theoretical model, the effective electric charge of addimers is estimated in the direction across dimer rows of the surface. The effective charge has a positive sign and does not exceed 15 units of the elementary charge in the temperature range of 1020–1120°C.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗