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At least 1,405 records · Page 78

Molecular dynamics simulation of Fe-Si alloys using a neural network machine learning potential

Interatomic potential development using machine learning (ML) approaches has attracted a lot of attention in recent years because these potentials can effectively describe the structural and dynamical properties of complex materials at the atomistic level. Here, in this work, we present the development of a neural network (NN) deep ML interatomic potential for Fe-Si alloys, and we demonstrate the effectiveness of the NN-ML potential in predicting the structures and energies of liquid and crystalline phases of Fe-Si alloys in comparison with the results from ab initio molecular dynamics simulations or experimental data. The developed NN-ML potential is also used to perform molecular dynamics simulations to study the structures of Fe-Si alloys with various compositions under rapid solidification conditions. The short-ranged orders in the rapidly solidified Fe-Si alloys are also analyzed by a cluster alignment method.

36 MATERIALS SCIENCE↗

Spin texture induced by non-magnetic doping and spin dynamics in 2D triangular lattice antiferromagnet h -Y(Mn,Al)O 3

Novel effects induced by nonmagnetic impurities in frustrated magnets and quantum spin liquid represent a highly nontrivial and interesting problem. A theoretical proposal of extended modulated spin structures induced by doping of such magnets, distinct from the well-known skyrmions has attracted significant interest. Here, we demonstrate that nonmagnetic impurities can produce such extended spin structures in h-YMnO 3 , a triangular antiferromagnet with noncollinear magnetic order. Using inelastic neutron scattering (INS), we measured the full dynamical structure factor in Al-doped h-YMnO 3 and confirmed the presence of magnon damping with a clear momentum dependence. Our theoretical calculations can reproduce the key features of the INS data, supporting the formation of the proposed spin textures. As such, our study provides the first experimental confirmation of the impurity-induced spin textures. It offers new insights and understanding of the impurity effects in a broad class of noncollinear magnetic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Motion of Drops on Surfaces with Wettability Gradients

A liquid drop present on a solid surface can move because of a gradient in wettability along the surface, as manifested by a gradient in the contact angle. The contact angle at a given point on the contact line between a solid and a liquid in a gaseous medium is the angle between the tangent planes to the liquid and the solid surfaces at that point and is measured within the liquid side, by convention. The motion of the drop occurs in the direction of increasing wettability. The cause of the motion is the net force exerted on the drop by the solid surface because of the variation of the contact angle around the periphery. This force causes acceleration of an initially stationary drop, and leads to its motion in the direction of decreasing contact angle. The nature of the motion is determined by the balance between the motivating force and the resisting hydrodynamic force from the solid surface and the surrounding gaseous medium. A wettability gradient can be chemically induced as shown by Chaudhury and Whitesides who provided unambiguous experimental evidence that drops can move in such gradients. The phenomenon can be important in heat transfer applications in low gravity, such as when condensation occurs on a surface. Daniel et al have demonstrated that the velocity of a drop on a surface due to a wettability gradient in the presence of condensation can be more than two orders of magnitude larger than that observed in the absence of condensation. In the present research program, we have begun to study the motion of a drop in a wettability gradient systematically using a model system. Our initial efforts will be restricted to a system in which no condensation occurs. The experiments are performed as follows. First, a rectangular strip of approximate dimensions 10 x 20 mm is cut out of a silicon wafer. The strip is cleaned thoroughly and its surface is exposed to the vapor from an alkylchlorosilane for a period lasting between one and two minutes inside a desiccator. This is done using an approximate line source of the vapor in the form of a string soaked in the alkylchlorosilane. Ordinarily, many fluids, including water, wet the surface of silicon quite well. This means that the contact angle is small. But the silanized surface resists wetting, with contact angles that are as large as 100 degs. Therefore, a gradient of wettability is formed on the silicon surface. The region near the string is highly hydrophobic, and the contact angle decreases gradually toward a small value at the hydrophilic end away from this region. The change in wettability occurs over a distance of several mm. The strip is placed on a platform within a Plexiglas cell. Drops of a suitable liquid are introduced on top of the strip near the hydrophobic end. An optical system attached to a video camera is trained on the drop so that images of the moving drop can be captured on videotape for subsequent analysis. We have performed preliminary experiments with water as well as ethylene glycol drops. Results from these experiments will be presented in the poster. Future plans include the refinement of the experimental system so as to permit images to be recorded from the side as well as the top, and the conduct of a systematic study in which the drop size is varied over a good range. Experiments will be conducted with different fluids so as to obtain the largest possible range of suitably defined Reynolds and Capillary numbers. Also, an effort will be initiated on theoretical modeling of this motion. The challenges in the development of the theoretical description lie in the proper analysis of the region in the vicinity of the contact line, as well as in the free boundary nature of the problem. It is known that continuum models assuming the no slip condition all the way to the contact line fail by predicting that the stress on the solid surface becomes singular as the contact line is approached. One approach for dealing with this issue has been to relax the no-slip boundary condition using the Navier model. Molecular dynamics simulations of the contact line region show that for a non-polar liquid on a solid surface, the no-slip boundary condition is in fact incorrect near the contact line. Furthermore, the same simulations also show that the usual relationship between stress and the rate of deformation breaks down in the vicinity of the contact line. In developing continuum theoretical models of the system, we shall accommodate this knowledge to the extent possible.

Subramanian, R. Shankar↗

A Dynamic Model for the Interaction Between an Insoluble Particle and an Advancing Solid/Liquid Interface

Most models that describe the interaction of an insoluble particle with an advancing solid-liquid interface are based on the assumption of steady state. However, as demonstrated by experimental work, the process does not reach steady state until the particle is pushed for a while by the interface. In this work, a dynamic mathematical model was developed. The dynamic model demonstrates that this interaction is essentially non-steady state and that steady state eventually occurs only when solidification is conducted at sub-critical velocities. The model was tested for three systems: aluminum-zirconia particles, succinonitrilepolystyrene particles, and biphenyl-glass particles. The calculated values for critical velocity of the pushing/engulfment transition were in same range with the experimental ones.

Catalina, A. V.↗

The relaxation behavior of supercooled and glassy imidacloprid

Employing dielectric spectroscopy, oscillatory shear rheology, and calorimetry, the present work explores the molecular dynamics of the widely used insecticide imidacloprid above and below its glass transition temperature. In its supercooled liquid regime, the applied techniques yield good agreement regarding the characteristic structural (alpha) relaxation times of this material. In addition, the generalized Gemant–DiMarzio–Bishop model provides a good conversion between the frequency-dependent dielectric and shear mechanical responses in its viscous state, allowing for an assessment of imidacloprid’s molecular hydrodynamic radius. In order to characterize the molecular dynamics in its glassy regime, we employ several approaches. These include the application of frequency–temperature superposition (FTS) to its isostructural dielectric and rheological responses as well as use of dielectric and calorimetric physical aging and the Adam–Gibbs–Vogel model. While the latter approach and dielectric FTS provide relaxation times that are close to each other, the other methods predict notably longer times that are closer to those reflecting a complete recovery of ergodicity. In conclusion, this seemingly conflicting dissimilarity demonstrates that the molecular dynamics of glassy imidacloprid strongly depends on its thermal history, with high relevance for the use of this insecticide as an active ingredient in technological applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Growth of Nanocrystal Superlattices from Liquid Crystals

The growth of superlattices (SLs) made from self-assembled nanocrystals (NCs) is a powerful method for creating new materials and gaining insight into fundamental molecular dynamics. Previous explorations of NCSL syntheses have mostly compared them to crystallization. However, NCSL synthesis has not broadly shown cooling crystallization from saturated solutions as a reversible crystallization–dissolution process. We demonstrate the reversible growth of NCSLs by dispersing NCs in liquid crystal (LC) “smart solvents,” and harnessing the transitions between the isotropic and nematic phases of the LCs. The growth mode and morphology can be tuned. Furthernore, this process is a model platform for studying crystallization and demonstrates great potential in manufacturing NCSLs as colloidal crystals through liquid-phase epitaxy or colloidal synthesis.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Direct observation of 3D atomic packing in monatomic amorphous materials

Liquids and solids are two fundamental states of matter. Although the structure of crystalline solids has long been solved by crystallography, our understanding of the 3D atomic structure of liquids and amorphous materials remained speculative. In 1952, Frank hypothesized that icosahedral order is the prevalent atomic motif in monatomic liquids. Over the past six decades, there have been a great deal of experimental, computational and theoretical studies to understand the structure of liquids and amorphous materials. A polytetrahedral packing model was proposed to explain the 3D atomic structure of monatomic liquids and amorphous materials, in which icosahedral order is a key feature. The icosahedral order has also been found to play an important role in the structure of metallic glasses and quasicrystals. Here we advance atomic electron tomography to determine for the first time the 3D atomic positions in monatomic amorphous materials, including a Ta thin film and two Pd nanoparticles. Despite the different chemical composition and synthesis methods, we observe that pentagonal bipyramids are the most abundant atomic motifs in these amorphous materials. Contrary to the traditional understanding, the pentagonal bipyramids do not assemble full icosahedra, but are closely connected with each other to form networks that extend to medium-range scale. Our molecular dynamic simulations, coupled with experimental results, further reveal that the 3D atomic structure of monatomic liquids is similar to the experimental amorphous material. Moreover, we find that the pentagonal bipyramid networks, prevalent in monatomic liquids, rapidly grow in size and form a fraction of full icosahedra during the quench from a liquid to a metallic glass state, providing a possible new picture of structural evolution through the glass transition.

Yuan, Yakun↗

Dynamic Measurements Near the Lambda-point in a Low-G Simulator on the Ground

The properties of liquid helium very near the lambda-transition in the presence of a heat current has received recent theoretical and experimental attention. In this regime, gravity induced pressure effects place severe constraints on the types of experiments that can be performed. A new experiment is described which largely overcomes these difficulties by magnetostrictively canceling gravity influences in the helium sample with a suitable magnetic coil. Design limitations of the technique and a discussion of proposed experiments is presented.

Israelsson, U. E.↗

Dynamic Measurements Near the Lambda-point in a Low-gravity Simulator on the Ground

The properties of liquid helium very near the lambda-transition in the presence of a heat current has received recent theoretical and experimental attention. In this regime, gravity induced pressure effects place severe constraints on the types of experiments that can be performed. A new experiment is described which largely overcomes these difficulties by magnetostrictively canceling gravity influences in the helium sample with a suitable magnetic coil. Design limitations of the technique and a discussion of proposed experiments is presented.

Israelsson, U. E.↗

A theoretical evaluation of rigid baffles in suppression of combustion instability

An analytical technique for the prediction of the effects of rigid baffles on the stability of liquid propellant combustors is presented. This analysis employs both two and three dimensional combustor models characterized by concentrated combustion sources at the chamber injector and a constant Mach number nozzle. An eigenfunction-matching method is used to solve the linearized partial differential equations describing the unsteady flow field for both models. Boundary layer corrections to this unsteady flow are used in a mechanical energy dissipation model to evaluate viscous and turbulence effects within the flow. An integral stability relationship is then employed to predict the decay rate of the oscillations. Results of this analysis agree qualitatively with experimental observations and show that sufficient dissipation exists to indicate that the proper mechanism of baffle damping is a fluid dynamic loss.

Combustion instability↗

Analytical Model for Steady Flow through a Finite Channel with One Porous Wall with Arbitrary Variable Suction or Injection

This paper presents an exact solution of two-dimensional laminar flow through a finite length channel with one porous wall. It improves upon previous solutions by (1) satisfying the no-slip boundary condition at the channel dead end, (2) adding a turbulent term to the porous wall boundary condition, (3) allowing for arbitrary variable suction or injection across the porous wall, and (4) model validation against new cryogenic liquid hydrogen and oxygen experimental data. Of particular interest in the current work is the modeling of cryogenic propellant flow through a porous liquid acquisition device (LAD) screen and channel inside a propellant tank. First, a detailed review of the literature is presented for previously attempted solutions to channel flow with one porous wall. Next, the governing equations, boundary conditions, and model assumptions are used to derive the analytical flow solution and present general model results for pressure and velocity fields within the channel. Then, the model solution is compared with horizontal LAD channel flow data in liquid oxygen as well as vertical LAD channel flow data in an inverted outflow configuration in liquid hydrogen. Model results are used to update the static cryogenic bubble point pressure model with a dynamic bubble point term which factors in enhanced convection and cooling at the screen during propellant outflow. Convective heat transfer at the LAD screen during outflow is also quantified by comparing model and data. The new analytical flow solution with the dynamic bubble point model is shown to compare well with available cryogenic experimental data

Navier Stokes Equations↗

Two-Phase Flow in Filters and Orifices: In preparation for Measurements on ISS Packed Bed Reactor Experiment-Water Recovery Series (PBRE-WRS)

Understanding the hydrodynamics of adiabatic two-phase flows in packed bed reactors offers numerous benefits. It enables the optimization of chemical reactions rates and products, crucial for pharmaceuticals and energy production industries. Additionally, this understanding aids in designing more efficient and compact reactors, reducing space and resource requirements. Insights gained from studying such flows in microgravity contribute to advancements of space technologies and the enhancement of our capabilities for undertaking future long duration safe, and sustainable space exploration missions. The Packed Bed Reactor Experiment-Water Recovery Series (PBRE-WRS) is a flight experiment planned for operation on the Microgravity Science Glove box (MSG) facility of the International Space Station (ISS). The objective of the experiment is to validate hydrodynamic models at a range of gas and liquid flow rates. The microgravity environment allows for measurement and observation of aspects of fluid dynamics that are unique when compared to observations made in full or partial gravity environments. The experiment consists of testing two-phase flow hydrodynamics in three different filters, four (4) orifices and one check valve test articles. The experiment utilizes the hardware of the previously flown PBRE and PBRE-2 with packed beds of different packings materials and sizes. The fluid system of the PBRE-WRS consists of a nitrogen gas delivery and water delivery subsystems. The gas delivery subsystem can accommodate two ranges of gas flow rates, just as for the water delivery system. The nitrogen gas loop is open whereas the water loop is closed. Gas is separated from the water using a gas-liquid phase separator which is located in the water delivery module. Preliminary results from ground testing show the pressure drop increasing at different rates with the liquid and gas flow rates in the Brine filter. In this work, a detailed system description is presented along with a summary of results from ground performance testing of different test sections in an end-to-end preflight testing campaign.

Packed Bed Reactor Experiment↗

Operando methods: A new era of electrochemistry

One of the grand challenges facing electrochemistry is to directly resolve the complex nature of (electro)catalyst active sites and capture real-time “movies” of reaction dynamics, i.e. “watching chemistry in action”. The need for such fundamental understanding has stimulated the development of operando/in situ methods, which have greatly enhanced our ability to identify activity descriptors of electrocatalysts and establish structure–property relationships of energy materials. Here, this review summarizes the frontiers of operando electrochemical liquid-cell scanning transmission electron microscopy and correlative synchrotron X-ray methods, which are complementary tools to comprehensively investigate reaction dynamics across multiple spatiotemporal scales. In an effort to encourage greater adoption of advanced operando methods by the general electrochemistry community, this review points out the need to benchmark electrochemistry in confined and heterogenous liquid environment with minimal beam-induced damage. We anticipate that multimodal operando methods will become indispensable for understanding interfacial reaction mechanisms for the broad chemistry and energy materials communities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Impacts of Synoptic-Scale Dynamics on Clouds and Radiation in High Southern Latitudes

High-latitudinal mixed-phase clouds significantly affect Earth's radiative balance. Observations of cloud and radiative properties from two field campaigns in the Southern Ocean and Antarctica were compared with two global climate model simulations. A cyclone compositing method was used to quantify “dynamics-cloud-radiation” relationships relative to the extratropical cyclone centers. Observations show larger asymmetry in cloud and radiative properties between western and eastern sectors at McMurdo compared with Macquarie Island. Most observed quantities at McMurdo are higher in the western (i.e., post-frontal) than the eastern (frontal) sector, including cloud fraction, liquid water path (LWP), net surface shortwave and longwave radiation (SW and LW), except for ice water path (IWP) being higher in the eastern sector. Here, the two models were found to overestimate cloud fraction and LWP at Macquarie Island but underestimate them at McMurdo Station. IWP is consistently underestimated at both locations, both sectors, and in all seasons. Biases of cloud fraction, LWP, and IWP are negatively correlated with SW biases and positively correlated with LW biases. The persistent negative IWP biases may have become one of the leading causes of radiative biases over the high southern latitudes, after correcting the underestimation of supercooled liquid water in the older model versions. By examining multi-scale factors from cloud microphysics to synoptic dynamics, this work will help increase the fidelity of climate simulations in this remote region.

58 GEOSCIENCES↗

Floquet Engineering of Interactions and Entanglement in Periodically Driven Rydberg Chains

Neutral atom arrays driven into Rydberg states constitute a promising approach for realizing programmable quantum systems. Enabled by strong interactions associated with Rydberg blockade, they allow for simulation of complex spin models and quantum dynamics. We introduce a new Floquet engineering technique for systems in the blockade regime that provides control over novel forms of interactions and entanglement dynamics in such systems. Our approach is based on time-dependent control of Rydberg laser detuning and leverages perturbations around periodic many-body trajectories as resources for operator spreading. These time-evolved operators are utilized as a basis for engineering interactions in the effective Hamiltonian describing the stroboscopic evolution. As an example, we show how our method can be used to engineer strong spin exchange, consistent with the blockade, in a one-dimensional chain, enabling the exploration of gapless Luttinger liquid phases. In addition, we demonstrate that combining gapless excitations with Rydberg blockade can lead to dynamic generation of large-scale multipartite entanglement. Experimental feasibility and possible generalizations are discussed.

Floquet systems↗

Investigation of Structure and Transport in Li-Doped Ionic Liquid Electrolytes: [pyr14][TFSI], [pyr13][FSI], [EMIM][BF4]

Ionic liquid electrolytes have been proposed as a means of improving the safety and cycling behavior of advanced lithium batteries; however, the properties of these electrolytes under high lithium doping are poorly understood. Here, we employ both polarizable molecular dynamics simulation and experiment to investigate the structure, thermodynamics and transport of three potential electrolytes, N-methyl-N-butylpyrrolidinium bis(trifluoromethylsufonyl)imide ([pyr14][TFSI]), N- methyl-N-propylpyrrolidinium bis(fluorosufonyl)imide ([pyr13][FSI]), and 1-ethyl-3-- methylimidazolium boron tetrafluoride ([EMIM][BF4]), as a function of Li (-) salt concentration and temperature. Structurally, Li(+) is shown to be solvated by three anion neighbors in [pyr14][TFSI] and four anion neighbors in both [pyr13][FSI] and [EMIM][BF4], and at all levels of xLi we find the presence of lithium aggregates. Furthermore, the computed density, diffusion, viscosity, and ionic conductivity show excellent agreement with experimental data. While the diffusion and viscosity exhibit a systematic decrease and increase, respectively, with increasing xLi, the contribution of Li(+) to ionic conductivity increases until reaching a saturation doping level of xLi 0.10. Comparatively, the Li(+) conductivity of [pyr14][TFSI] is an order of magnitude lower than that of the other liquids, which range between 0.1-0.3 mScm. The differences in Li(+) transport are reflected in the residence times of Li(+) with the anions, which are revealed to be much larger for [pyr14][TFSI] (up to 100 ns at the highest doping levels) than in either [EMIM][BF4] or [pyr13][FSI]. Finally, we comment on the relative kinetics of Li(+) transport in each liquid and we present strong evidence for transport through anion exchange (hopping) as opposed to the net motion of Li(+) with its solvation shell (vehicular).

ionic liquids↗

Mare basalt petrogenesis in a dynamic moon

An hypothesis for mare basalt petrogenesis is presented. In the proposed model, both high- and low-Ti mare basalts are produced by partial melting and hybridization at depth accompanied by equilibrium between the hybrid liquids and the local olivine-pyroxenite residuum. The energy source for mare basalt formation is ultimately provided by radiogenic heating in the primordial lunar interior. The proposed dynamic model explains similarities in the Mg/(Mg+Fe) ratios and Cr2O3 contents of high-Ti and low-Ti basalts and avoids thermal problems inherent in previous models.

Kesson, S. E.↗

Ion Dissociation Dynamics in an Aqueous Premelting Layer

Using molecular dynamics simulations and methods of importance sampling, we study the thermodynamics and dynamics of sodium chloride in the aqueous premelting layer formed spontaneously at the interface between ice and its vapor. We uncover a hierarchy of time scales that characterize the relaxation dynamics of this system, spanning the picoseconds of ionic motion to the tens or hundreds of nanoseconds associated with fluctuations of the liquid-crystal interface in their presence. We find that ions distort both local interfaces, incurring restoring forces that result in the ions preferentially residing in the middle of the layer. While ion pair dissociation is thermodynamically favorable, these structural and dynamic effects cause its rate to vary by over an order of magnitude through the layer, with a maximum rate significantly depressed from the corresponding bulk value. The solvation environment of ions in the premelting layer is distinct from that in a bulk liquid, being dominated by slow reorganization of water molecules and a water structure intermediate between ice and its melt.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗