Structure and Stability of SnO[subscript 2] Nanocrystals and Surface-Bound Water Species
Abstract not provided
Wang, Hsiu-Wen↗
SEARCH · Engineering Papers
Results for “GROUP DYNAMICS”
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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Using magnetic dynamics to measure the spin gap in a candidate Kitaev material
Spin-orbit entangled materials have attracted widespread interest due to the novel magnetic phenomena arising from the interplay between spin-orbit coupling and electronic correlations. However, the intricate nature of spin interactions within Kiteav materials complicates the precise measurement of low-energy spin excitations. Using Na 2 Co 2 TeO 6 as an example, we study these low-energy spin excitations using the time-resolved resonant elastic x-ray scattering (tr-REXS). Our observations unveil remarkably slow spin dynamics at the magnetic peak, whose recovery timescale is several nanoseconds. This timescale aligns with the extrapolated spin gap of ~1 μeV, obtained by density matrix renormalization group (DMRG) simulations in the thermodynamic limit. The consistency demonstrates the efficacy of tr-REXS in discerning low-energy spin gaps inaccessible to conventional spectroscopic techniques.
36 MATERIALS SCIENCE↗
Evaluating the stability and activity of dilute Cu-based alloys for electrochemical CO 2 reduction
Cu-based catalysts currently offer the most promising route to actively and selectively produce value-added chemicals via electrochemical reduction of CO 2 (eCO 2 R); yet further improvements are required for their wide-scale deployment in carbon mitigation efforts. Here, we systematically investigate a family of dilute Cu-based alloys to explore their viability as active and selective catalysts for eCO 2 R through a combined theoretical–experimental approach. Using a quantum–classical modeling approach that accounts for dynamic solvation effects, we assess the stability and activity of model single-atom catalysts under eCO 2 R conditions. Our calculations identify that the presence of eCO2R intermediates, such as CO*, H*, and OH*, may dynamically influence the local catalyst surface composition. Additionally, we identify through binding energy descriptors of the CO*, CHO*, and OCCO* dimer intermediates that certain elements, such as group 13 elements (B, Al, and Ga), enhance the selectivity of C 2+ species relative to pure Cu by facilitating CO dimerization. The theoretical work is corroborated by preliminary testing of eCO 2 R activity and selectivity of candidate dilute Cu-based alloy catalyst films prepared by electron beam evaporation in a zero-gap gas diffusion electrode-based reactor. Of all studied alloys, dilute CuAl was found to be the most active and selective toward C 2+ products like ethylene, consistent with the theoretical predictions. Finally, we attribute the improved performance of dilute CuAl alloys to more favorable dimerization reaction energetics of bound CO species relative to that on pure Cu. In a broader context, the results presented here demonstrate the power of our simulation framework in terms of rational catalyst design.
30 DIRECT ENERGY CONVERSION↗
Ultrafast sorting: Excimeric π–π stacking distinguishes pyrene-N-methylacetamide isomers on the ultrafast time scale
Pyrene based molecules are inclined to form excimers through self-association upon photoexcitation. In this work, the pyrene core is functionalized with N-methylacetamide group at the position 1 or 2, to develop pyren-1-methylacetamide (PyMA1) and pyren-2- methylacetamide (PyMA2), respectively. The introduction of methylacetamide group was believed to help having hydrogen bonded excimers in close aggregation. Upon photoexcitation, PyMA1 and PyMA2, at 1.0mM in toluene, have formed predominantly static and dynamic excimers, respectively. The transient absorption (TA) measurements over fs-ps regime (fs-TA) showed that the formation of static excimers is an ultrafast process (~560fs) whereas, the dynamic excimers formed in much slower time scale (~65ps). Finally, single crystal X-ray diffraction studies show that for PyMA2 the overlap between the pyrene moieties (~42%) are better than PyMA1 (~17%) in ground state at 80K, which also reflected in the respective lifetimes and population percentages of excimers.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Cation reordering instead of phase transitions: Origins and implications of contrasting lithiation mechanisms in 1D ζ- and 2D α-V 2 O 5
Substantial improvements in cycle life, rate performance, accessible voltage, and reversible capacity are required to realize the promise of Li-ion batteries in full measure. Here, we have examined insertion electrodes of the same composition (V 2 O 5 ) prepared according to the same electrode specifications and comprising particles with similar dimensions and geometries that differ only in terms of their atomic connectivity and crystal structure, specifically two-dimensional (2D) layered α-V 2 O 5 that crystallizes in an orthorhombic space group and one-dimensional (1D) tunnel-structured ζ-V 2 O 5 crystallized in a monoclinic space group. By using particles of similar dimensions, we have disentangled the role of specific structural motifs and atomistic diffusion pathways in affecting electrochemical performance by mapping the dynamical evolution of lithiation-induced structural modifications using ex situ scanning transmission X-ray microscopy, operando synchrotron X-ray diffraction measurements, and phase-field modeling. We find the operation of sharply divergent mechanisms to accommodate increasing concentrations of Li-ions: a series of distortive phase transformations that result in puckering and expansion of interlayer spacing in layered α-V 2 O 5 , as compared with cation reordering along interstitial sites in tunnel-structured ζ-V 2 O 5 . By alleviating distortive phase transformations, the ζ-V 2 O 5 cathode shows reduced voltage hysteresis, increased Li-ion diffusivity, alleviation of stress gradients, and improved capacity retention. The findings demonstrate that alternative lithiation mechanisms can be accessed in metastable compounds by dint of their reconfigured atomic connectivity and can unlock substantially improved electrochemical performance not accessible in the thermodynamically stable phase.
25 ENERGY STORAGE↗
Efficiency of fermionic quantum distillation
Here, we present a time-dependent density-matrix renormalization group investigation of the quantum distillation process within the Fermi-Hubbard model on a quasi-one-dimensional ladder geometry. The term distillation refers to the dynamical, spatial separation of singlons and doublons in the sudden expansion of interacting particles in an optical lattice, i.e., the release of a cloud of atoms from a trapping potential. Remarkably, quantum distillation can lead to a contraction of the doublon cloud, resulting in an increased density of the doublons in the core region compared to the initial state. As a main result, we show that this phenomenon is not limited to chains that were previously studied. Interestingly, there are additional dynamical processes on the two-leg ladder such as density oscillations and self-trapping of defects that lead to a less efficient distillation process. An investigation of the time evolution starting from product states provides an explanation for this behavior. Initial product states are also considered since in optical lattice experiments, such states are often used as the initial setup. We propose configurations that lead to a fast and efficient quantum distillation.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Neutrino energy transport in weak decoupling and big bang nucleosynthesis
In this study, we calculate the evolution of the early universe through the epochs of weak decoupling, weak freeze-out and big bang nucleosynthesis (BBN) by simultaneously coupling a full strong, electromagnetic, and weak nuclear reaction network with a multienergy group Boltzmann neutrino energy transport scheme. The modular structure of our code provides the ability to dissect the relative contributions of each process responsible for evolving the dynamics of the early universe in the absence of neutrino flavor oscillations. Such an approach allows a detailed accounting of the evolution of the νe, ν¯e, νμ, ν¯μ, ντ, ν¯τ energy distribution functions alongside and self-consistently with the nuclear reactions and entropy/heat generation and flow between the neutrino and photon/electron/positron/baryon plasma components. This calculation reveals nonlinear feedback in the time evolution of neutrino distribution functions and plasma thermodynamic conditions (e.g., electron-positron pair densities), with implications for the phasing between scale factor and plasma temperature; the neutron-to-proton ratio; light-element abundance histories; and the cosmological parameter N eff . We find that our approach of following the time development of neutrino spectral distortions and concomitant entropy production and extraction from the plasma results in changes in the computed value of the BBN deuterium yield. For example, for particular implementations of quantum corrections in plasma thermodynamics, our calculations show a 0.4% increase in deuterium. These changes are potentially significant in the context of anticipated improvements in observational and nuclear physics uncertainties.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Relaxation of vacuum energy in q-theory
The q-theory formalism aims to describe the thermodynamics and dynamics of the deep quantum vacuum. The thermodynamics leads to an exact cancellation of the quantum-field zero-point-energies in equilibrium, which partly solves the main cosmological constant problem. But, with reversible dynamics, the spatially flat Friedmann–Robertson–Walker universe asymptotically approaches the Minkowski vacuum only if the Big Bang already started out in an initial equilibrium state. Here, we extend q-theory by introducing dissipation from irreversible processes. Neglecting the possible instability of a de-Sitter vacuum, we obtain different scenarios with either a de-Sitter asymptote or collapse to a final singularity. The Minkowski asymptote still requires fine-tuning of the initial conditions. This suggests that, within the q-theory approach, the decay of the de-Sitter vacuum is a necessary condition for the dynamical solution of the cosmological constant problem.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Investigation of Dynamics in BMIM TFSA Ionic Liquid through Variable Temperature and Pressure NMR Relaxometry and Diffusometry
A comprehensive variable temperature, pressure and frequency multinuclear ( 1 H, 2 H, and 19 F) magnetic resonance study was undertaken on selectively deuterated 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)amide (BMIM TFSA) ionic liquid isotopologues. This study builds on our earlier investigation of the effects of increasing alkyl chain length on diffusion and dynamics in imidazolium-based TFSA ionic liquids. Fast field cycling 1 H T 1 data revealed multiple modes of motion. Through calculation of diffusion coefficient (D) values and activation energies, the low- and high-field regimes were assigned to the translational and reorientation dynamics respectively. Variable-pressure 2 H T 1 measurements reveal site-dependent interactions in the cation with strengths in the order MD 3 > CD 3 > CD 2 , indicating dissimilarities in the electric field gradients along the alkyl chain, with the CD 2 sites having the largest gradient. Additionally, the α saturation effect in T 1 vs. P was observed for all three sites, suggesting significant reduction of the short-range rapid reorientational dynamics. This reduction was also deduced from the variable pressure 1 H T 1 data, which showed an approach to saturation for both the methyl and butyl group terminal methyl sites. Pressure-dependent D measurements show independent motions for both cations and anions, with the cations having greater D values over the entire pressure range.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
First principles molecular dynamics maps out complete mineral surface acidity landscape
In “Interfacial structures and acidity constants (pKa) of goethite from first principles molecular dynamics simulations,” authors Y. Zhang, X. Lui, J. Cheng, and X. Lu apply First Principles molecular dynamics (FPMD, also called Density Functional Theory MD, DFT/MD, or ab initio MD, AIMD), to evaluable the complete set of acidity constants (pK a ) of the hydroxyl groups on the most prominent goethite crystal facets. The pK a of these OH and OH$^+_2$ groups are compared with available data from the multisite complexation (MUSIC) model traditionally used to estimate pK a on mineral surfaces. The authors have presented eloquent rationale for the importance and implications of understanding goethite acidity constants in room temperature geochemistry settings. In this paper, I focus on the computational aspects, the strengths of FPMD, and its possibilities.
58 GEOSCIENCES↗
A Dynamically Polarized Solid Target for CLAS12
The 12 GeV physics program in Hall B at Jefferson Lab will be centered on the newly commissioned, high acceptance spectrometer CLAS12 and will utilize a variety of nuclear targets, including a dynamically polarized solid target for experiments on longitudinally polarized protons, deuterons, and lithium nuclei. The target, under construction in a collaborative effort between the Jefferson Lab Target Group, Christopher Newport University, Old Dominion University, and the University of Virginia, is designed with a number of innovative features. These include multiple target cells for reduced systematic uncertainties, internal superconducting shim coils to adjust the polarizing magnetic field, and a 1 K evaporation refrigerator with an integrated load lock system for the target samples. The current status of the system's design, construction, and various R&D efforts are described.
Keith, Christopher↗
Howard University Energy Expert Systems Institute Summer Program (EESI)
Howard University, under the auspices of the Center for Energy Systems and Controls runs the Energy Expert Systems Institute (EESI) summer outreach program for high school/pre-college minority students. The main objectives are to introduce precollege minority students to research in the power industry using modern state-of-the-art technology such as Expert Systems, Fuzzy Logic and Artificial Neural Networks; to involve minority students in space power management, systems and failure diagnosis; to generate interest in career options in electrical engineering; and to experience problem-solving in a teamwork environment consisting of faculty, senior research associates and graduate students. For five weeks the students are exposed not only to the exciting experience of college life, but also to the inspiring field of engineering, especially electrical engineering. The program consists of lectures in the fundamentals of engineering, mathematics, communication skills and computer skills. The projects are divided into mini and major. Topics for the 1995 mini projects were Expert Systems for the Electric Bus and Breast Cancer Detection. Topics on the major projects include Hybrid Electric Vehicle, Solar Dynamics and Distribution Automation. On the final day, designated as 'EESI Day' the students did oral presentations of their projects and prizes were awarded to the best group. The program began in the summer of 1993. The reaction from the students has been very positive. The program also arranges field trips to special places of interest such as the NASA Goddard Space Center.
Momoh, James A.↗
Tele-Supervised Adaptive Ocean Sensor Fleet
The Tele-supervised Adaptive Ocean Sensor Fleet (TAOSF) is a multi-robot science exploration architecture and system that uses a group of robotic boats (the Ocean-Atmosphere Sensor Integration System, or OASIS) to enable in-situ study of ocean surface and subsurface characteristics and the dynamics of such ocean phenomena as coastal pollutants, oil spills, hurricanes, or harmful algal blooms (HABs). The OASIS boats are extended- deployment, autonomous ocean surface vehicles. The TAOSF architecture provides an integrated approach to multi-vehicle coordination and sliding human-vehicle autonomy. One feature of TAOSF is the adaptive re-planning of the activities of the OASIS vessels based on sensor input ( smart sensing) and sensorial coordination among multiple assets. The architecture also incorporates Web-based communications that permit control of the assets over long distances and the sharing of data with remote experts. Autonomous hazard and assistance detection allows the automatic identification of hazards that require human intervention to ensure the safety and integrity of the robotic vehicles, or of science data that require human interpretation and response. Also, the architecture is designed for science analysis of acquired data in order to perform an initial onboard assessment of the presence of specific science signatures of immediate interest. TAOSF integrates and extends five subsystems developed by the participating institutions: Emergent Space Tech - nol ogies, Wallops Flight Facility, NASA s Goddard Space Flight Center (GSFC), Carnegie Mellon University, and Jet Propulsion Laboratory (JPL). The OASIS Autonomous Surface Vehicle (ASV) system, which includes the vessels as well as the land-based control and communications infrastructure developed for them, controls the hardware of each platform (sensors, actuators, etc.), and also provides a low-level waypoint navigation capability. The Multi-Platform Simulation Environment from GSFC is a surrogate for the OASIS ASV system and allows for independent development and testing of higher-level software components. The Platform Communicator acts as a proxy for both actual and simulated platforms. It translates platform-independent messages from the higher control systems to the device-dependent communication protocols. This enables the higher-level control systems to interact identically with heterogeneous actual or simulated platforms.
Lefes, Alberto↗
Recent Results of a New Microwave SQUID Multiplexer
We are developing a proof-of-concept microwave SQUID multiplexer containing four SQUIDs coupled to GHz frequency resonant circuits and fed with a single microwave readout line. The resonators are half-wave coplanar waveguide sections and are similar to the structures used for the microwave kinetic inductance detectors developed in our group. Optimal values for the interdigital gap capacitors were determined to maximize the sensitivity of the transmitted and reflected microwave signal with respect to changes in the dynamic resistance of the SQUID. The dc current-bias line for the SQUID has an in-line inductive high frequency filter to minimize coupling between the bias line and resonator. A high frequency modulation scheme is proposed to eliminate the need for individual flux biasing of the SQUIDs, which extends the dynamic range of the readout. In this scheme a common modulation signal is imposed on each SQUID and the received signal is demodulated at one and two times the modulation frequency to maintain sensitivity at any flux state. We present the recent results of the microwave SQUID multiplexer system operating at a readout frequency range of 10 - 11GHz.
superconducting quantum interference device (SQUID↗
Advanced Libya-4 radiometric and atmospheric characterization utilizing MODIS and VIIRS full-scan reflective solar band measurements
The NASA Clouds and the Earth's Radiant Energy System (CERES) project provides observed flux and cloud products to the climate science community. The CERES instruments, along with the MODIS and VIIRS imagers, are onboard the Terra, Aqua, NPP, and NOAA20 satellites. In order to produce seamless multi-platform integrated products, long-term sensor stability and inter-calibration are required. Inter-calibration between sensors within the same sun-synchronous orbit relies on Earth invariant targets because simultaneous nadir overpasses are not possible. To facilitate inter-calibration efforts, the CERES Imager and Geostationary Calibration Group (IGCG) has improved the Libya-4 target characterization. Improvements include full scan angle characterization to enable daily observations, clear-sky identification using individual scan angle dynamic spatial homogeneity thresholds, and atmospheric corrections. The water vapor correction was found to be effective across the full scan, whereas the ozone and aerosol corrections were less effective. The atmospheric-corrected normalized radiance temporal fluctuations are similar across scan angles, spectral bands, and between the MODIS and VIIRS imagers, suggesting that the fluctuations are a result of the natural variability of the Libya-4 surface reflectance. The Libya-4 surface variability is more than likely caused by changes in the prevailing winds that alter sand dune orientation and resulting shadows. The full-scan-imager atmosphere and angle corrected reflected solar band radiance trend standard errors are between 0.6% and 1.0%, and for near-nadir observations, are between 0.5% and 0.8%. The advanced characterization suggests that the Libya-4 short-term surface reflectance anomalies may need to be considered for imager stability monitoring and inter-calibration efforts.
Libya-4 Pseudo-invariant Calibration Site↗
Electronic Tuning of Photoexcited Dynamics in Heteroleptic Cu(I) Complex Photosensitizers
Photoexcited dynamics of heteroleptic Cu(I) complexes as noble-metal-free photosensitizers are closely intertwined with the nature of their ligands. By utilizing ultrafast optical and X-ray transient absorption spectroscopies, we characterized a new set of heteroleptic Cu(I) complexes [Cu(PPh 3 )( 2 )(BPy R )] + (R = CH 3 , H, Br to COOCH 3 ), with an increase in the electron-withdrawing ability of the functional group (R). Here we found that after the transient photooxidation of Cu(I) to Cu(II), the increasing electron-withdrawing ability of R barely affects the internal conversion (IC) (e.g., Jahn-taller (JT) distortion) between singlet MLCT states. However, it does accelerate the dynamics of intersystem crossing (ISC) between singlet and triplet MLCT states and the subsequent decay from the triplet MLCT state to the ground state. The associated lifetime constants are reduced by up to 300%. Our understanding of the photoexcited dynamics in heteroleptic Cu(I) complexes through ligand electronic tuning provides valuable insight into the rational design of efficient Cu(I) complex photosensitizers.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Effects of water on the mechanical properties of silica glass using molecular dynamics
Understanding the effects of water on the mechanical properties of silica glass is important for many applications of silicate glasses. In this study, the effects of water on both elastic and plastic properties of pure silica glass are investigated. The introduction of molecular water leads to an increase of Young's modulus of silica glass at low water content, while hydroxyl exhibits an opposite effect. Although hydroxyl groups decrease both strength and fracture toughness of the glass via destructing the silica network connectivity, molecular water undermines these properties by effectively driving the silica network to a “strained” configuration in absence of external stress. The water effect can be characterized in terms of the change of Si-O bond length and Si-O-Si bond angle. The plateau in the stress-strain curves of silica with the existence of molecular water in compact tension is associated with the Si-O bond breaking followed by formation of silanol groups. Furthermore, the introduction of molecular water lowers the critical tensile stress where the plateau occurs.
36 MATERIALS SCIENCE↗
Stochastic dynamics of small ensembles of non-processive molecular motors: The parallel cluster model
Non-processive molecular motors have to work together in ensembles in order to generate appreciable levels of force or movement. In skeletal muscle, for example, hundreds of myosin II molecules cooperate in thick filaments. In non-muscle cells, by contrast, small groups with few tens of non-muscle myosin II motors contribute to essential cellular processes such as transport, shape changes, or mechanosensing. Here we introduce a detailed and analytically tractable model for this important situation. Using a three-state crossbridge model for the myosin II motor cycle and exploiting the assumptions of fast power stroke kinetics and equal load sharing between motors in equivalent states, we reduce the stochastic reaction network to a one-step master equation for the binding and unbinding dynamics (parallel cluster model) and derive the rules for ensemble movement. We find that for constant external load, ensemble dynamics is strongly shaped by the catch bond character of myosin II, which leads to an increase of the fraction of bound motors under load and thus to firm attachment even for small ensembles. This adaptation to load results in a concave force-velocity relation described by a Hill relation. For external load provided by a linear spring, myosin II ensembles dynamically adjust themselves towards an isometric state with constant average position and load. The dynamics of the ensembles is now determined mainly by the distribution of motors over the different kinds of bound states. For increasing stiffness of the external spring, there is a sharp transition beyond which myosin II can no longer perform the power stroke. Slow unbinding from the pre-power-stroke state protects the ensembles against detachment.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗