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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 1,099 records · Page 61

Elucidating molecular scale interactions underlying the freezing behavior of salt solutions in silica nanopores

Elucidating the influence of nanoscale confinement on the freezing behavior of salt solutions is of fundamental interest to environmental security and materials science and engineering. Specific structural information such as the coordination environment of ions in confined aqueous medium, effects on the extended hexagonal network of water molecules and their mutual non-bonding interactions in confinement are sparse in the literature along with the change in the dynamical characteristics of water in the presence of ions. To address these knowledge gaps, the current study is focused on investigating the influence of reduced dimensionality arising from nanoscale confinement on the structural evolution of salt solutions on freezing and the associated fluid–surface interactions. In this regard, operando wide-angle X-ray scattering (WAXS) measurements and classical molecular dynamics (MD) simulations are conducted with water and 0.5 M CaCl 2 , MgCl 2 and KCl solutions confined in 4 nm sized SBA-15 silica pores upon cooling from 300 K to 200 K. The freezing point of the salt solutions is depressed to 235 K which is about 10 K lower than that of confined water. The translational dynamics of confined salt solutions indicates shifts in the fragile-to-strong dynamical crossover to a lower temperature compared to pure water. The strong electrostatic attraction between the cations and the surrounding water molecules contributes to the freezing point depression in confined salt solutions. These insights unlock the molecular-scale basis and mechanisms underlying the freezing behavior of confined salt solutions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ansatz-Free Hamiltonian Learning with Heisenberg-Limited Scaling

Learning the unknown interactions that govern a quantum system is crucial for quantum information processing, device benchmarking, and quantum sensing. The problem, known as Hamiltonian learning, is well understood under the assumption that interactions are local, but this assumption may not hold for arbitrary Hamiltonians. Previous methods all require high-order inverse polynomial dependency with precision, unable to surpass the standard quantum limit and reach the gold-standard Heisenberg-limited scaling. Whether Heisenberg-limited Hamiltonian learning is possible without prior assumptions about the interaction structures, a challenge we term ansatz-free Hamiltonian learning , remains an open question. In this work, we present a quantum algorithm to learn arbitrary sparse Hamiltonians without any structure constraints using only black-box queries of the system’s real-time evolution and minimal digital controls to attain Heisenberg-limited scaling in estimation error. Our method is also resilient to state-preparation-and-measurement errors, enhancing its practical feasibility. We numerically demonstrate our ansatz-free protocol for learning physical Hamiltonians and validating analog quantum simulations, benchmarking our performance against the state-of-the-art Heisenberg-limited learning approach. Moreover, we establish a fundamental trade-off between total evolution time and quantum control on learning arbitrary interactions, revealing the intrinsic interplay between controllability and total evolution-time complexity for any learning algorithm. These results pave the way for further exploration into Heisenberg-limited Hamiltonian learning in complex quantum systems under minimal assumptions, potentially enabling new benchmarking and verification protocols.

machine learning↗

Experimental study of three-dimensional CO 2 -water drainage and fracture-matrix interactions in fractured porous media

Estimation of CO 2 storage capacity in fractured porous reservoirs requires a better understanding of the CO 2 -water flow fundamentals in fracture-matrix systems. There are few core-flood experiments on three-dimensional CO 2 -water drainage in a fracture-matrix system, yet none have examined the impacts of the capillary continuity of fractures and fracture-matrix interactions. In this study, twelve drainage experiments were conducted in four fracture-matrix columns, each comprising a vertical stack of a cylindrical rock core, a filter paper serving as an analogue to a horizontal fracture, and a ceramic plate. Here, the core sample was surrounded by open space at the top and circumferential sides to model fractures, allowing for 3-D CO 2 -water drainage in the rock core and displaced water draining across the horizontal fracture. X-ray computed tomography was conducted to visualize the dynamic invasion/drainage processes in four rock core samples showing contrasts in anisotropy, permeability, and heterogeneity. Experimental results show (1) the equilibrium CO 2 saturations in the rock matrix vary from 0.10 to 0.60 at controlled capillary pressures up to 200 kPa, (2) the CO 2 saturations in the matrix increase with water saturation in the horizontal fracture resulting in better capillary continuity for water to drain across the fracture, and (3) the fracture water saturation can be enhanced by the non-uniform fracture capillary pressure and countercurrent flow of CO 2 and water across the fracture-matrix interface. In the case of high fracture water saturation, matrix CO 2 saturation largely depends on matrix anisotropy and heterogeneity. The core-scale experimental results contribute to understand the fracture-matrix interactions and CO 2 storage efficiency in fractured porous media.

54 ENVIRONMENTAL SCIENCES↗

Spin–orbit configuration interaction study of spectral properties of PbO

Relativistic calculations of the structural and spectral properties of the PbO molecule can provide fundamental information about the importance of a proper treatment of angular momentum coupling among electrons in order to achieve accurate computational results for spectral properties. Specifically, the nature of these couplings in PbO is expected to be intermediate between the LS- and jj-coupling limits because of its light/heavy element composition. This article reports potential energy curves, transition energies, electric dipole transition moments, permanent dipole moments and spectroscopic constants of PbO calculated using a multireference single plus double excitations spin–orbit configuration interaction approach in the context of relativistic effective core potentials and their concomitant spin–orbit coupling operators. The calculated results are in general agreement with both available experimental results as well as earlier calculations. New values for properties of excited states are also reported. It is noteworthy that certain properties show larger deviations from previous calculations. Furthermore, these deviations are attributed to direct and indirect relativistic effects resulting from diatomic electron–electron angular momentum coupling effects, which are included consistently in the calculations reported herein.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

HPC4Mfg with ACS

Distillation in the chemical industry accounts for roughly 10% of energy use in the U.S. While porous mass separating agents (MSAs) appear capable of achieving the same separations for a fraction of the energy, the fundamental lack of a well-understood relationship between the behavior of fluid mixtures confined in MSA pores and the selectivity of MSA-based processes presents a major barrier to their widespread industrial application. This work is the first study to systematically and self-consistently explore a range of parameters describing various molecule-material interactions in MSA-based separations. Through high performance computing (HPC), this study has yielded a fundamental understanding of the influence of confined fluid behavior on selectivity. The results also serve as a knowledge base for subsequent investigations needed to transform the framework for rational design of MSA-based separation processes. This will significantly reduce the energy required for separations central to chemical manufacturing.

36 MATERIALS SCIENCE↗

Fire as a fundamental ecological process: Research advances and frontiers

Fire is a powerful ecological and evolutionary force that regulates organismal traits, population sizes, species interactions, community composition, carbon and nutrient cycling and ecosystem function. It also presents a rapidly growing societal challenge, due to both increasingly destructive wildfires and fire exclusion in fire–dependent ecosystems. As an ecological process, fire integrates complex feedbacks among biological, social and geophysical processes, requiring coordination across several fields and scales of study. Here, we describe the diversity of ways in which fire operates as a fundamental ecological and evolutionary process on Earth. We explore research priorities in six categories of fire ecology: (a) characteristics of fire regimes, (b) changing fire regimes, (c) fire effects on above–ground ecology, (d) fire effects on below–ground ecology, (e) fire behaviour and (f) fire ecology modelling. We identify three emergent themes: the need to study fire across temporal scales, to assess the mechanisms underlying a variety of ecological feedbacks involving fire and to improve representation of fire in a range of modelling contexts. As fire regimes and our relationships with fire continue to change, prioritizing these research areas will facilitate understanding of the ecological causes and consequences of future fires and rethinking fire management alternatives.

54 ENVIRONMENTAL SCIENCES↗

Studies in High Energy Heavy Ion Nuclear Physics

This close-out report covers the period 1994 - 2015 for DOE grant DE-FG02-94ER40845 with the University of Texas at Austin. The research was concerned with studies of the strong nuclear force and properties of nuclear matter under extreme conditions of temperature and density which far exceed that in atomic nuclei. Such extreme conditions are briefly created (for about 10 trillionths of a trillionth of a second) during head-on collisions of large atomic nuclei (e.g. gold) colliding at speeds very close to the speed-of-light. The collisions produce thousands of subatomic particles, many of which are detected in our experiment called STAR at the Relativistic Heavy-Ion Collider at the Brookhaven National Lab in New York. The goal of our research is to learn how the strong nuclear force and its fundamental particles (quarks and gluons) behave in extreme conditions similar to that of the early Universe when it was about 1 micro-second old, and in the cores of very dense neutron stars. To learn anything new about the matter which exists for such a very short amount of time requires carefully designed probes. In our research we focused on two such probes, one being short-lived resonance particles and the other using correlations between pairs of the detected particles. Resonances are short-lived particles created in the collision, which interact with the surrounding matter, and which break apart, or "decay" into more stable particles which survive long enough to be seen in our detectors. The dependence of resonance properties on the conditions in the collision system permit tests of theoretical models and improve our understanding. Dynamical interactions in the matter also leave imprints on the final, outgoing particle distributions measured in the experiment. In particular, angular correlations between pairs of particles can be related to the fundamental strong force as it behaves in the hot, dense matter. Studying correlations as a function of experimentally controlled conditions of the collisions provides another test of theory. Our results provide unambiguous evidence that the briefly existing hot, dense matter has strong effects on the measurements and indicate that the matter is best described in terms of the fundamental quarks and gluons, that its internal interactions are surprisingly strong, and that new and never before seen strong interaction processes are occurring which remain to be explained theoretically. To enable these studies our group has also made substantial contributions to the detection capabilities of the STAR experiment. These contributions were to the electronics required to "read out" the weak electrical signals from the detectors and transfer the raw data to offline computers for processing. Although this experimental program is now concluded, the resonance and correlation results we have extracted from the raw collision data will continue to challenge and perhaps guide theoretical developments of the strong nuclear force for many years to come.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Transport of colloidal particles in microscopic porous medium analogs with surface charge heterogeneity: experiments and fundamental role of single-bead deposition

Understanding colloid transport in subsurface environments is challenging due to complex interactions between colloids, ground water, and porous media over several length scales. Here, we study the transport of colloidal particles through bead-assembled microfluidic porous media analogs (PMAs) with surface charge heterogeneity. The pore-scale dynamics of colloidal particle deposition were measured, as well as the breakthrough curves (BTC) and retention profiles (RP) of deposited colloidal particles at the scale of the entire PMA. From pore-scale experiments, the maximum surface coverage (?max = 0.51) was measured directly, from which the surface blocking function and deposition coefficient (kpore = 3.56 s-1) were obtained. Using these pore-scale parameters, the transport of colloidal particles was modeled using a one-dimensional advection-dispersion equation under the assumption of irreversible adsorption between oppositely charged beads and colloids, showing good agreement with experimental data. This work presents a new approach to fabricate chemically heterogeneous porous media in a microfluidic device that enables direct measurements of pore-scale colloidal deposition. The approach allows a quantitative prediction of colloidal breakthrough and retention via coupling of direct measurements and an advection-dispersion-deposition model.

Guo, Yang↗

Scoping assessments of ATF impact on late–stage accident progression including molten core-concrete interaction

Simple scoping models that can be used to evaluate ATF performance under severe accident conditions have been developed. The methodology provides a fundamental technical basis (a.k.a. metric) based on the thermodynamic boundary for evaluating performance relative to that of traditional Zr-based claddings. The initial focus in this study was on UO 2 fuel with the advanced claddings 310 SS, D9, FeCrAl, and SiC. The evaluation considered only energy release with concurrent combustible gas production from fuel–cladding–coolant interactions and, separately, molten core–concrete interactions at high temperatures. Other important phenomenological effects that can influence the rate and extent of cladding decomposition (e.g., eutectic interactions, degradation of other core constituents) were not addressed. For the cladding types addressed, potential combustible gas production under both in-vessel and ex-vessel conditions was similar to that for Zr. However, exothermic energy release from cladding oxidation was substantially less for iron-based alloys (by at least a factor of 4), and modestly less (by ~20%) for SiC. Data on SiC-clad UO 2 fuel performance under severe accident conditions are sparse in the literature; thus, assumptions on the nature of the cladding decomposition process were made in order to perform this initial screening evaluation. Furthermore, experimental data for this system under severe accident conditions is needed for a proper evaluation and comparison to iron-based claddings.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Light-induced Kondo-like exciton-spin interaction in neodymium(II) doped hybrid perovskite

Abstract Tuning the properties of a pair of entangled electron and hole in a light-induced exciton is a fundamentally intriguing inquiry for quantum science. Here, using semiconducting hybrid perovskite as an exploratory platform, we discover that Nd 2+ -doped CH 3 NH 3 PbI 3 (MAPbI 3 ) perovskite exhibits a Kondo-like exciton-spin interaction under cryogenic and photoexcitation conditions. The feedback to such interaction between excitons in perovskite and the localized spins in Nd 2+ is observed as notably prolonged carrier lifetimes measured by time-resolved photoluminescence, ~10 times to that of pristine MAPbI 3 without Nd 2+ dopant. From a mechanistic standpoint, such extended charge separation states are the consequence of the trap state enabled by the antiferromagnetic exchange interaction between the light-induced exciton and the localized 4 f spins of the Nd 2+ in the proximity. Importantly, this Kondo-like exciton-spin interaction can be modulated by either increasing Nd 2+ doping concentration that enhances the coupling between the exciton and Nd 2+ 4 f spins as evidenced by elongated carrier lifetime, or by using an external magnetic field that can nullify the spin-dependent exchange interaction therein due to the unified orientations of Nd 2+ spin angular momentum, thereby leading to exciton recombination at the dynamics comparable to pristine MAPbI 3 .

36 MATERIALS SCIENCE↗

First-Principles Study of Interaction between Molecules and Lewis Acid Zeolites Manipulated by Injection of Energized Charge Carriers

Metal dopants in Lewis acid zeolites can be applied to manipulate the interaction between the active sites and molecular reactants. However, only a few elements can be introduced into the zeolite framework to generate strong Lewis acid sites. In this study, we propose an alternative approach to tune the interaction between zeolite and molecules by introducing energized charge carriers that are photoexcited in a complex of plasmonic metal and zeolites. Here, through density functional theory (DFT) calculations, we show that although the energized electrons do not impact the adsorption of ammonia, which is used as a probe molecule, on Zr- and Si-BEA, ammonia’s heat of adsorption can be reduced up to 60% on Sn-BEA and 20% on Ti-BEA, respectively, because of the localized population of the electrons at the Sn and Ti center. This most pronounced effect in Sn-BEA is attributed to the Sn-induced midgap states and the strong electronegativity of Sn atoms. In contrast, the energized holes can strengthen the interaction between zeolites and ammonia by at least 10%. Particularly, if an energized hole is present in the system, the heat of adsorption of ammonia within Si-BEA can increase 3-fold, shifting from weak to moderate interaction. We find that, similar to closed sites, the effect of energized charge carriers can also be extended to open sites of Lewis acid zeolites. Our study provides fundamental insights for unlocking the potentials of integrating plasmonic metals with zeolites and brings an additional degree of control to tune the interfacial interaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

RADIAL STELLAR PULSATION AND THREE-DIMENSIONAL CONVECTION. IV. FULL AMPLITUDE THREE-DIMENSIONAL SOLUTIONS

Three-dimensional hydrodynamic simulations of full amplitude RR Lyrae stars have been computed for several models across the instability strip. The three-dimensional nature of the calculations allows convection to be treated without reference to a phenomenological approach such as the local mixing length theory. Specifically, the time-dependent interaction of large-scale eddies and radial pulsation is controlled by conservation laws, while the effects of smaller convective eddies are simulated by an eddy viscosity model. The light amplitudes for these calculations are quite similar to those of our previous two-dimensional calculations in the middle of the instability strip, but somewhat lower near the red edge, the fundamental blue edge, and for the one first overtone model we computed. The time-dependent interaction between the radial pulsation and the convective energy transport is essentially the same in three dimensions as it is in two dimensions. There are some differences between the light curves of the two- and three-dimensional simulations, particularly during decreasing light. Reasons for the differences, both numerical and physical, are explored.

79 ASTRONOMY AND ASTROPHYSICS↗

Stress measurement in thick plates using nonlinear ultrasonics

In this paper the interaction between nonlinear ultrasonic characteristics and stress state of complex loaded thick steel plates using fundamental theory of nonlinear ultrasonics is investigated in order to measure the stress state at a given cross section. The measurement concept is based on phased array placement of ultrasonic transmitter-receiver to scan three angles of a given cross section using Rayleigh waves. The change in the ultrasonic data in thick steel plates is influenced by normal and shear stresses; therefore, three measurements are needed to solve the equations simultaneously. Different thickness plates are studied in order to understand the interaction of Rayleigh wave penetration depth and shear stress. The purpose is that as the thickness becomes smaller, the shear stress becomes negligible at the angled measurement. For thicker cross section, shear stress becomes influential if the depth of penetration of Rayleigh wave is greater than the half of the thickness. The influences of plate thickness and ultrasonic frequency on the identification of stress tensor are numerically studied in 3D structural geometry and Murnaghan material model. The experimental component of this study includes uniaxial loading of the plate while measuring ultrasonic wave at three directions (perpendicular, parallel and angled to the loading direction). Instead of rotating transmitter-receiver pair for each test, a device capable of measuring the three angles is designed.

42 ENGINEERING↗

Negative Ion Formation in Complex Heavy Systems

The project’s primary objective is to gain a fundamental theoretical understanding of the near-threshold electron attachment mechanism in low energy electron elastic scattering from complex heavy systems through the calculation of integral and differential cross sections and extract reliable electron affinities (EAs). The complex angular momentum (CAM), also known as Regge-pole methodology wherein is fully embedded the crucial electron-electron correlations and the core polarization interaction, is used for the investigations. Regge trajectories allow us to probe electron attachment at the fundamental level near threshold, thereby uncovering new manifestations, including the mechanism of nanocatalysis, and determine reliable EAs. Low-energy electron elastic scattering total cross sections (TCSs) for the lanthanide and actinide atoms and the fullerene molecules are calculated. From the TCSs ground, metastable and excited states anionic binding energies (BEs) are extracted and compared with the available measured and/or calculated EAs. Significantly, our calculated ground state anionic BEs correspond to the theoretically challenging to calculate EAs and they are used to assess the reliability of existing EAs. Doubly charged negative ions of atoms and molecules are proposed as novel tunable catalysts and demonstrated in the oxidation of water into peroxide. Negatively charged fullerene molecules are used to catalyze water oxidation to peroxide and water synthesis from H 2 and O 2 as well. Violation of time-reversal and particle-hole symmetries in strongly correlated Fermi systems are reviewed with the collaboration involving the International Laboratory of Fermi Condensation.

74 ATOMIC AND MOLECULAR PHYSICS↗

Broken symmetries and excitation spectra of interacting electrons in partially filled Landau levels

Interacting electrons in flat bands give rise to a variety of quantum phases. One fundamental aspect of such states is the ordering of the various flavours – such as spin or valley – that the electrons can undergo and the excitation spectrum of the broken symmetry states that they form. These properties cannot be probed directly with electrical transport measurements. The zeroth Landau level of monolayer graphene with four-fold spin-valley degeneracy is a model system for such investigations, but the nature of its broken symmetry states – particularly at partial fillings – is still not understood. Here, in this study, we demonstrate a non-invasive spectroscopic technique with a scanning tunneling microscope and use it to perform measurements of the valley polarization of the electronic wavefunctions and their excitation spectrum in the partially filled zeroth Landau level of graphene. We can extract information such as the strength of Haldane pseudopotentials that characterize the repulsive interactions underlying the fractional quantum states. Our experiments also demonstrate that fractional quantum Hall phases are built upon broken symmetry states that persist at partial filling. Our experimental approach quantifies the valley phase diagram of the partially filled Landau level as a model flat band platform which is applicable to other graphene-based electronic systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Proton spin structure and generalized polarizabilities in the strong quantum chromodynamics regime

The strong interaction is not well understood at low energies or for interactions with low momentum transfer. Chiral perturbation theory gives testable predictions for the nucleonic generalized polarizabilities, which are fundamental quantities describing the nucleon’s response to an external field. We report a measurement of the proton’s generalized spin polarizabilities extracted with a polarized electron beam and a polarized solid ammonia target in the region where chiral perturbation theory is expected to be valid. The investigated structure function g2 characterizes the internal spin structure of the proton. From its moments, we extract the longitudinal–transverse spin polarizability δLT and twist-3 matrix element and polarizability d2¯. Our results provide discriminating power between existing chiral perturbation theory calculations and will help provide a better understanding of this strong quantum chromodynamics regime.

Ruth, D↗

Ecological Principles and Guidelines for Managing the Use of Land

The many ways that people have used and managed land throughout history has emerged as a primary cause of land-cover change around the world. Thus, land use and land management increasingly represent a fundamental source of change in the global environment. Despite their global importance, however, many decisions about the management and use of land are made with scant attention to ecological impacts. Thus, ecologists' knowledge of the functioning of Earth's ecosystems is needed to broaden the scientific basis of decisions on land use and management. In response to this need, the Ecological Society of America established a committee to examine the ways that land-use decisions are made and the ways that ecologists could help inform those decisions. This paper reports the scientific findings of that committee. Five principles of ecological science have particular implications for land use and can assure that fundamental processes of Earth's ecosystems are sustained. These ecological principles deal with time, species, place, dis- turbance, and the landscape. The recognition that ecological processes occur within a temporal setting and change over time is fundamental to analyzing the effects of land use. In addition, individual species and networks of interacting species have strong and far-reaching effects on ecological processes. Furthermore, each site or region has a unique set of organisms and abiotic conditions influencing and constraining ecological processes. Distur- bances are important and ubiquitous ecological events whose effects may strongly influence population, com- munity, and ecosystem dynamics. Finally, the size, shape, and spatial relationships of habitat patches on the landscape affect the structure and function of ecosystems. The responses of the land to changes in use and management by people depend on expressions of these fundamental principles in nature. These principles dictate several guidelines for land use. The guidelines give practical rules of thumb for incorporating ecological principles into land-use decision making. These guidelines suggest that land managers should: (1) examine impacts of local decisions in a regional context, (2) plan for long-term change and unexpected events, (3) preserve rare landscape elements and associated species, (4) avoid land uses that deplete natural resources, (5) retain large contiguous or connected areas that contain critical habitats, (6) minimize the intro- duction and spread of nonnative species, (7) avoid or compensate for the effects of development on ecological processes, and (8) implement land-use and management practices that are compatible with the natural potential of the area. Decision makers and citizens are encouraged to consider these guidelines and to include ecological per- spectives in choices on how land is used and managed. The guidelines suggest actions required to develop the science needed by land managers.

Ecology↗

The homogeneous mixing of MgO and H 2 O at extreme conditions

Investigating water worlds presents a unique opportunity to understand the fundamental processes of planetary formation and evolution. One key aspect is characterizing the interactions between water and rock under the pressures and temperatures present within these worlds. Investigating the conditions for the homogeneous mixing of these materials is imperative to characterizing bulk properties and evolution of water-rich exoplanets. Here, in this study, we use density functional molecular dynamics simulations to study MgO-H 2 O mixtures at high pressure–temperature conditions where H 2 O occurs in solid, superionic, or liquid form. MgO, the representative rocky material, can be either solid or liquid. We start from 500 K at 120 GPa, increasing the temperature step by step up to 8000 K. By inspection, we determine the temperature at which MgO-HO homogeneously mix in our simulations. At 6000 K and 174 GPa is when we find the system to homogeneously mix. This heat-until-it-mixes approach provides us with an upper bound on the temperature for the mixing of MgO and H 2 O. We find that homogeneous mixing occurs at sufficiently low temperatures to be relevant for the collisional growth of a water-rich planet.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗