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At least 973 records · Page 54

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DOE OSTI2021

Probing Metastable Domain Dynamics via Automated Experimentation in Piezoresponse Force Microscopy

The dynamics of complex topological defects in ferroelectric materials is explored using automated experimentation in piezoresponse force microscopy. Specifically, a complex trigger system (i.e., “FerroBot”) is employed to study metastable domain-wall dynamics in Pb 0.6 Sr 0.4 TiO 3 thin films. Several regimes of superdomain wall dynamics have been identified, including smooth domain-wall motion and significant reconfiguration of the domain structures. We have further demonstrated that microscopic mechanisms of the domain-wall dynamics can be identified; i.e., domain-wall bending can be separated from irreversible domain reconfiguration regimes. In conjunction, phase-field modeling was used to corroborate the observed mechanisms. As such, the observed superdomain dynamics can provide a model system for classical ferroelectric dynamics, much like how colloidal crystals provide a model system for atomic and molecular systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

High-throughput nuclear resonance time domain interferometry using annular slits

Nuclear resonance time domain interferometry (NR-TDI) is used to study the slow dynamics of liquids (that do not require Mössbauer isotopes) at atomic and molecular length scales. Here the TDI method of using a stationary two-line magnetized 57 Fe foil as a source and a stationary single-line stainless steel foil analyzer is employed. The new technique of adding an annular slit in front of a single silicon avalanche photodiode detector enables a wide range of momentum transfers (1 to 100 nm -1 by varying the distance between the annular slits and sample) with a high count rate of up to 160 Hz with a Δ q resolution of ±1.7 nm -1 at q = 14 nm -1 . The sensitivity of this method in determining relaxation times is quantified and discussed. The Kohlrausch–Williams–Watts (KWW) model was used to extract relaxation times for glycerol. These relaxation times give insight into the dynamics of the electron density fluctuations of glycerol as a function of temperature and momentum transfers.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Comparing ab initio and quantum-kinetic approaches to electron transport in warm dense matter

Accurate knowledge of the electronic transport properties of warm dense matter is one of the main concerns of research in high-energy-density physics. Three modern approaches with vastly different levels of fidelity are reviewed and compared: the Kubo–Greenwood (KG) approach based on density-functional-theory molecular dynamics simulations (QMD), quantum kinetic theory based on average-atom models, and time-dependent density functional theory. Throughout, emphasis is placed on the connection between static properties of the electrons (e.g., density of states) and transport properties. Overall, it is found that whenever the conduction electrons can be modeled as being nearly free, fair to excellent agreement is found between QMD and kinetic theory approaches. Such a circumstance is required for modeling warm dense matter as a plasma of ions and free electrons, which is assumed in most kinetic theory approaches. The sensitivity of transport properties to the electronic structure is further highlighted by comparing different exchange–correlation approximations in QMD and KG calculations. It is found that the inclusion of exact exchange via thermal hybrid functionals can make a pronounced impact on electrical and thermal conduction in warm dense matter. We also investigate dynamic screening physics via kinetic theory and time-dependent density functional theory calculations of the mean free path of an electron in a hot dense plasma. In sum, we identify three axes along which to make progress in predicting electron transport in warm dense matter.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Neural network potential for Zr–Rh system by machine learning

Zr–Rh metallic glass has enabled its many applications in vehicle parts, sports equipment and so on due to its outstanding performance in mechanical property, but the knowledge of the microstructure determining the superb mechanical property remains yet insufficient. Here, we develop a deep neural network potential of Zr–Rh system by using machine learning, which breaks the dilemma between the accuracy and efficiency in molecular dynamics simulations, and greatly improves the simulation scale in both space and time. Here, the results show that the structural features obtained from the neural network method are in good agreement with the cases in ab initio molecular dynamics simulations. Furthermore, we build a large model of 5400 atoms to explore the influences of simulated size and cooling rate on the melt-quenching process of Zr 77 Rh 23 . Our study lays a foundation for exploring the complex structures in amorphous Zr 77 Rh 23 , which is of great significance for the design and practical application.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Optomechanical self-organization in a mesoscopic atom array

Increasing the number of particles in a system often leads to qualitative changes in its properties, such as breaking of symmetries and the appearance of phase transitions. This renders a macroscopic system fundamentally different from its individual microscopic constituents. Lying between these extremes, mesoscopic systems exhibit microscopic fluctuations that influence behaviour on longer length scales, leading to critical phenomena and dynamics. Therefore, tracing the properties of well-controlled mesoscopic systems can help bridge the gap between an exact description of few-body microscopic systems and the emergent description of many-body systems. Here we explore the mesoscopic signatures of an optomechanical self-organization phase transition using arrays of cold atoms inside an optical cavity. By precisely engineering atom–cavity interactions, we reveal how critical behaviour depends on the atom number, identify characteristic dynamical behaviours in the self-organized regime and observe a finite optomechanical susceptibility at the critical point. These findings advance our understanding of particle-number- and time-resolved properties of phase transitions in mesoscopic systems.

Atomic and molecular interactions with photons↗

DOE OSTI2024

Effect of CO 2 on the water slip flow at silica surfaces for nanometer slit pores of talc

In our previous study, Molecular Dynamics (MD) simulated water flow with no dissolved gas in nanometer slit pores of the hydrophobic talc surfaces revealed a slip length of about 0.5 nm, which is close to the size of “water exclusion zone” but much less than experimental slip length. Atomic Force Microscopy (AFM) imaging confirmed the presence of pancake shape nanobubbles at the hydrophobic talc (001) surface (size from tens to hundreds of nanometers). The effect of CO 2 on water slip flow in talc nanopores is reported to reveal the importance of dissolved gas for confined fluid flow. MD simulated 7 nm CO 2 nanobubbles were found to attach and spread at the talc (001) surface, consistent with the AFM observation. Simulated CO 2 saturated water flow in the slit pores of talc (001) surfaces predicted the generation of CO 2 nanobubbles at the end of the slit pore, due to the stabilization of a CO 2 film at the talc (001) surfaces and a water barrier at the edge surfaces of talc. A “critical thickness” of about 1.5 nm was found for CO 2 nanobubbles to be stabilized at the end of the talc (001) surface. With 1.5 nm CO 2 nanobubbles at the talc (001) surface of a 6 nm slit pore, a water slip length of 1.8 nm was determined. Furthermore, the nanometer slit pore simulations with dissolved CO 2 in water revealed an increased slip length. It is expected that an increased slip length value would be found with an increased CO 2 film thickness.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules

Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, the spectral congestion of valence photoelectron spectra sets fundamental limits to the complexity of systems that can be studied, and the delocalization of valence electron wave functions blurs the spatial origin of the photoelectron wave packet. Using attosecond x-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: The photoelectron spectra remain atomlike, the measurements become element specific, and the observed scattering dynamics originate from a pointlike source when multicenter interference effects are negligible. We exploit these unique features to reveal the effects of changing functional groups (C-H vs N) and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N−1⁢𝑠 and C−1⁢𝑠 core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wave function with the replacement of C-H groups by N atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter.

Ji, Jia-Bao [Eidgenoessische Technische Hochschule↗

DOE OSTI2021

Unraveling the intrinsic atomic physics behind x-ray absorption line shifts in warm dense silicon plasmas

Here, we present a novel free-energy density functional theory (DFT)-based methodology for optical property calculations of warm dense matter to cover a wide range of thermodynamic conditions and photon energies including the entire x-ray range. It uses Mermin–Kohn–Sham density functional theory with exchange-correlation (XC) thermal effects taken into account via a fully temperature dependent generalized gradient approximation XC functional. The methodology incorporates a combination of the ab initio molecular dynamics (AIMD) snapshotted Kubo–Greenwood optic data with a single-atom in simulation cell calculations to close the photon energy gap between the L and K edges and extend the K-edge tail toward many-keV photon energies. This gap arises in the standard scheme due to a prohibitively large number of bands required for the Kubo–Greenwood calculations with AIMD snapshots. Kubo–Greenwood data on snapshots provide an accurate description of optic properties at low photon frequencies slightly beyond the L-edge and x-ray absorption near edges structure (XANES) spectra, while data from periodic calculations with single atoms cover the tail regions beyond the edges. To demonstrate its applicability to mid-Z materials where the standard DFT-based approach is not computationally feasible, we have applied it to opacity calculations of warm dense silicon plasmas. These first-principles calculations revealed a very interesting phenomon of red-to-blue shift in K–L (1s → 2p) and K-edge absorptions along both isotherm and isochore, which are absent in most continuum-lowering models of traditional plasma physics. This new physics phenomenon can be attributed to the underlying competition between the screening of deeply bound core electrons and the screening of outer-shell electrons caused by warm-dense-plasma conditions. We further demonstrate that the ratio of 1s → 2p to the K-edge x-ray absorptions can be used to characterize warm-dense-plasma conditions. Eventually, based on our absorption calculations, we have established a first-principles opacity table (FPOT) for silicon in a wide range of material densities and temperatures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Large-scale atomistic studies of sliding friction in polycrystalline aluminum interfaces

In this work, we discuss large-scale non-equilibrium molecular dynamics (NEMD) simulations of ductile metal sliding comprising up to 1.8 × 10 9 atoms over time scales of 100 ns. The results of these simulations have identified a variety of physical mechanisms that are important in determining the steady-state frictional force for a wide range of velocities at compressed metal–metal interfaces. These include grain growth and refinement, the evolution of large plastic strains and strain rates, material mixing, and melting. These phenomena can be included in a strain, strain rate, and grain size model that gives good agreement with the NEMD simulations and can be applied to macroscopic continua.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

LDRD 226360 Final Project Report: Simulated X-ray Diffraction and Machine Learning for Optimizing Dynamic Experiment Analysis

This report is the final documentation for the one-year LDRD project 226360: Simulated X-ray Diffraction and Machine Learning for Optimizing Dynamic Experiment Analysis. As Sandia has successfully developed in-house X-ray diffraction tools for study of atomic structure in experiments, it has become increasingly important to develop computational analysis methods to support these experiments. When dynamically compressed lattices and orientations are not known a priori, the identification requires a cumbersome and sometimes intractable search of possible final states. These final states can include phase transition, deformation and mixed/evolving states. Our work consists of three parts: (1) development of an XRD simulation tool and use of traditional data science methods to match XRD patterns to experiments; (2) development of ML-based models capable of decomposing and identifying the lattice and orientation components of multicomponent experimental diffraction patterns; and (3) conducting experiments which showcase these new analysis tools in the study of phase transition mechanisms. Our target material has been cadmium sulfide, which exhibits complex orientation-dependent phase transformation mechanisms. In our current one-year LDRD, we have begun the analysis of high-quality c-axis CdS diffraction data from DCS and Thor experiments, which had until recently eluded orientation identification.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Rapid activation of non-oriented mechanophores via shock loading and spallation

Mechanophores (MPs), stimuli-responsive molecules that respond chromatically to mechanochemical reactions, are important for understanding the coupling between mechanics and chemistry as well as in engineering applications. However, the atomic-level understanding of their activation originates from gas phase studies or under simple linear elongation forces directly on molecules or polymer chains containing MPs. The effect of many-body distortions, pervasive in condensed-phase applications, is not understood. Therefore, we performed large-scale molecular dynamics (MD) simulations of a poly(methyl methacrylate)-spiropyran copolymer under dynamic mechanical loading and studied the activation of the MP under various conditions from dynamical compression to tension during unloading. Detailed analysis of the all-atom MD trajectories shows that the MP blocks experience significant many-body intramolecular distortion that can significantly decrease the activation barrier as compared with when deformation rates are slow relative to molecular relaxation time scales. Here we find that the reactivity of MPs under material compression states is governed by many-body effects of intramolecular torsions, whereas under tension, the reactions are governed by tensile stresses.

36 MATERIALS SCIENCE↗

NASA NTRSDate not supplied

Semi-Empirical Interatomic Potential for Large-Scale Molecular Dynamics Simulation of Metal-Oxide Systems

Classical molecular dynamics (MD) simulation can be applied to systems containing billions of atoms during times up to microseconds. However, utilization of a large-scale MD simulation requires reliable but computationally cheap interatomic potentials. In the case of metallic systems, embedded atom method (EAM) and Finnis-Sinclair (FS) potentials are the reasonable choices, but their development for multicomponent alloys is a challenge. Addition of oxygen atoms makes the problem of developing semi-empirical potentials even more difficult because the long-range Coulomb interaction cannot be neglected, and different atoms have different charges which vary during MD relaxation such that a charge equilibration procedure should be applied every MD step. As results researchers tend to avoid simulating metal-oxide systems. In this talk, a new Finnis-Sinclair (FS) Ni-Co-Cr potential will be presented. Special attention will be paid to reproducing of the element melting temperatures and clustering. Next, a charge transfer ionic potential (CTIP) developed to simulate the NiO properties will be presented. This potential utilizes the Ni FS potential and accounts for the Coulomb interaction in the vicinity of oxygen atoms. Fitting of the CTIP parameters and FS potential functions describing the interaction with oxygen atoms to the available experimental and ab initio data will be discussed. Results of MD simulation of interaction of NiO particles with dislocations in Ni will be shown.

molecular dynamics simulation↗

DOE OSTI2021

Irradiation-enhanced diffusion and diffusion-limited creep in U 3 Si 2

U 3 Si 2 is an advanced fuel candidate due to its relatively high fissile density and attractive thermal properties. Compared to standard UO 2 fuel, there are significant data gaps for the thermophysical and thermomechanical properties of U 3 Si 2 . Point defect concentrations and mobilities under irradiation govern a number of important fuel performance properties, such as creep and fission gas release. In this work, we utilized density functional theory (DFT) data to inform a cluster dynamics framework to predict point defect concentrations in U 3 Si 2 under irradiation. Molecular dynamics (MD) simulations were used to examine the contribution of atomic mixing during ballistic cascades to diffusion, as well as the diffusivity of U and Si at grain boundaries. These atomic scale models for diffusivity were then used to inform a creep model based on bulk (Nabarro-Herring) and grain boundary (Coble) diffusional creep, and climb-limited dislocation creep. The model compares well against available experimental data and has been implemented in the BISON fuel performance code. Finally, a demonstration case using simple power profiles has been carried out, showing that negligible creep occurs due to the low temperatures experienced by U 3 Si 2 in-reactor, a consequence of its high thermal conductivity.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Advances in ultrafast gas-phase x-ray scattering

Recent developments of x-ray free electron lasers and pulsed electron sources have enabled ultrafast scattering to become an increasingly powerful tool for exploring molecular dynamics. Here, this article describes our recent experimental and methodological advances in ultrafast gas-phase x-ray scattering experiments at the LCLS. A re-designed short-pathlength windowless diffractometer is coupled with careful optimization of sample density and independent normalization of x-ray intensity fluctuations to provide gas-phase scattering patterns with exceptionally high signal-to-noise ratios. These advances, coupled with careful geometry optimization and data treatment, provide both ground- and excited-state signals in excellent agreement with high level ab initio total scattering patterns.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2023

Tuning anisotropic bonding via chemistry and pressure in layered pnictides and chalcogenides (Final Report)

The overarching goal of this research program, as originally delineated in the proposal “Tuning anisotropic bonding via chemistry and pressure in layered pnictides and chalcogenides” was to develop a predictive, chemistry-driven understanding of the impact of the phonon behavior on thermal properties of bulk layered materials. At finite temperatures, atomic vibrations (phonons) strongly impact the thermodynamics, thermal and electrical transport, and phase-switching properties of functional materials. In particular, soft phonon modes and strongly anharmonic potentials can have spectacular consequences, including structural phase transitions (for example in ferroelectrics and phase-change memory materials), metal-insulator transitions, and extreme thermal resistance preventing heat propagation. Bulk materials with highly-anisotropic bonding may provide unique strategies to induce soft-phonon modes and lattice instabilities. Recently, increasingly detailed investigations of the lattice dynamics in layered materials have been made possible by the advent of first-principles phonon calculations and advanced characterization techniques based on neutron and X-ray scattering. However, due to the lack of studies in which composition and bonding character are systematically varied, there are still fundamental questions regarding the impacts of anisotropic bonding and anharmonicity on lattice stability and thermal transport. One of the major goals of this research program is therefore to address this gap by coherently tuning bonding anisotropy and anharmonicity across families of related compounds. Such approaches have revealed new strategies for exploiting structural anisotropy in quasi-1D and 2D bulk materials to obtain tailored functional properties. This project systematically explored the lattice dynamics, phase stability, and transport properties in bulk layered materials by using both composition and applied pressure to tune the degree of bonding anisotropy and anharmonicity. To accomplish this work, we combined i) single-crystal growth of key material systems with tunable anisotropy, ii) in-situ high-temperature/high-pressure characterization of structure and phonons to probe bonding anisotropy and anharmonicity, including state-of-the-art inelastic X-ray scattering (IXS) and inelastic neutron scattering (INS), and iii) first-principles simulations leveraging large-scale computing to identify the fundamental origins of the observed effects, by relating atomic structure and dynamics to electronic orbital interactions. Finally, we modeled and verified the impact of the phonon behavior on thermal transport to identify new strategies for a-priori design of thermal conductivity. Our integrated collaborative approach helped to systematically unravel the effects of anisotropy and bonding anharmonicity on phonon transport, thermodynamics, and thermal properties of complex anisotropic materials.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2022

Tuning anisotropic bonding via chemistry and pressure in layered pnictides and chalcogenides. Final Report

36 MATERIALS SCIENCE↗

DOE OSTI2024

Variations in proton transfer pathways and energetics on pristine and defect-rich quartz surfaces in water: Insights into the bimodal acidities of quartz

Hypothesis. Understanding the mechanisms of proton transfer on quartz surfaces in water is critical for a range of processes in geochemical, environmental, and materials sciences. The wide range of surface acidities (>9 pKa units) found on the ubiquitous mineral quartz is caused by the structural variations of surface silanol groups. Molecular scale simulations provide essential tools for elucidating the origin of site-specific surface acidities. Simulations. Here, we used density-functional tight-binding-based molecular dynamics combined with rare-event metadynamics simulations to probe the mechanisms of deprotonation reactions from ten representative surface silanol groups found on both pristine and defect-rich quartz (1 0 1) surfaces with Si vacancies. Findings. The results show that deprotonation is a highly dynamic process where both the surface hydroxyls and bridging oxygen atoms serve as the proton acceptors, in addition to water. Deprotonation of embedded silanols through intrasurface proton transfer exhibited lower pKa values with less H-bond participation and higher energy barriers, suggesting a new mechanism to explain the bimodal acidity observed on quartz surface. Defect sites, recently shown to comprise a significant portion of the quartz (1 0 1) surface, diversify the coordination and local H-bonding environments of the surface silanols, changing both the deprotonation pathways and energetics, leading to a wider range of pKa values (2.4 to 11.5) than that observed on pristine quartz surface (10.4 and 12.1).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Solution Structure and Scaling Laws of Cylindrical and Tapered Bottlebrush Polymers

Bottlebrush polymers are a unique class of macromolecular architectures with a plethora of potential industrial and pharmaceutical applications that critically depend on the bottlebrush shape and dimensions. Here, a systematic series of 12 cylindrical and 12 cone-shaped (tapered) bottlebrush polymers with poly(tert-butyl acrylate) (PtBA) or polystyrene (PS) side chains were synthesized using the sequential addition of macromonomers ring-opening metathesis polymerization (SAM-ROMP) grafting-through method. Small-angle neutron scattering (SANS) studies on dilute solutions of the two types of bottlebrush polymers provided noninvasive characterization of their structural dimensions and chain conformations. Simulated SANS traces, generated using coarse-grained molecular dynamics simulations, reproduced the distinctive features observed in the experimental SANS signals and provided necessary validation for data modeling. The combined analysis of experimental and simulated SANS signals yielded key structural and conformational parameters, including the bottlebrush radius, length, and Kuhn length as well as the excluded volume parameter and the correlation length of the polymer side chains. Importantly, the obtained structural parameters followed well-defined scaling laws as a function of the backbone and side chain degrees of polymerization, as predicted by mean field theories. In conclusion, these findings provide clear experimental and computational evidence of the interdependence of structural and conformational properties in an important class of polymer architectures.

36 MATERIALS SCIENCE↗