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At least 883 records · Page 49

Photoinduced iodide repulsion and halides-demixing in layered perovskites

Mixing halides in metal halide perovskites (MHPs) is an effective approach for adjusting the MHPs bandgap for applications in tandem solar cells. However, mixed-halide (MH-) MHPs undergo light-induced phase segregation (LIPS) under continuous illumination. Therefore, understanding the mechanism of LIPS is necessary for developing stable MH-MHPs. Here, we investigated LIPS in layered (L) MHPs and discovered a critical role of spacer cations in LIPS. Through probing chemical changes of LIPS, we unveil light-induced iodide repulsion and the formation of Br-rich-phase in illuminated regions during LIPS. This discovery also gives insight into the LIPS process in three-dimensional (3D) MHPs. By further investigating LIPS in 3D MHPs, we reveal that LIPS induces not only the formation of Br-rich and I-rich domains but also an overall change of halide distribution along the film thickness direction. Furthermore, LIPS is more significant in bulk due to a larger population of photogenerated charge carriers. Overall, this study reveals the chemical mechanism of LIPS in MHPs and its potential effect on device performance, offering insight into understanding the LIPS mechanism and improving the stability of MHPs.

36 MATERIALS SCIENCE↗

2D/3D Visual Tracker for Rover Mast

A visual-tracker computer program controls an articulated mast on a Mars rover to keep a designated feature (a target) in view while the rover drives toward the target, avoiding obstacles. Several prior visual-tracker programs have been tested on rover platforms; most require very small and well-estimated motion between consecutive image frames a requirement that is not realistic for a rover on rough terrain. The present visual-tracker program is designed to handle large image motions that lead to significant changes in feature geometry and photometry between frames. When a point is selected in one of the images acquired from stereoscopic cameras on the mast, a stereo triangulation algorithm computes a three-dimensional (3D) location for the target. As the rover moves, its body-mounted cameras feed images to a visual-odometry algorithm, which tracks two-dimensional (2D) corner features and computes their old and new 3D locations. The algorithm rejects points, the 3D motions of which are inconsistent with a rigid-world constraint, and then computes the apparent change in the rover pose (i.e., translation and rotation). The mast pan and tilt angles needed to keep the target centered in the field-of-view of the cameras (thereby minimizing the area over which the 2D-tracking algorithm must operate) are computed from the estimated change in the rover pose, the 3D position of the target feature, and a model of kinematics of the mast. If the motion between the consecutive frames is still large (i.e., 3D tracking was unsuccessful), an adaptive view-based matching technique is applied to the new image. This technique uses correlation-based template matching, in which a feature template is scaled by the ratio between the depth in the original template and the depth of pixels in the new image. This is repeated over the entire search window and the best correlation results indicate the appropriate match. The program could be a core for building application programs for systems that require coordination of vision and robotic motion.

Bajracharya, Max↗

How correlations change the magnetic structure factor of the kagome Hubbard model

The kagome Hubbard model (KHM) is a paradigmatic example of a frustrated two-dimensional model. While its strongly correlated regime, described by a Heisenberg model, is of topical interest due to its enigmatic prospective spin-liquid ground state, the weakly and moderately correlated regimes remain largely unexplored. Motivated by the rapidly growing number of metallic kagome materials (e.g., Mn 3 Sn, Fe 3 Sn 2 , FeSn, Co 3 Sn 2 S 2 , Gd 3 Ru 4 Al 12 , and AV 3 Sb 5 with A = K, Rb, Cs), here we study the respective regimes of the KHM by means of three complementary numerical methods: the dynamical mean-field theory, the dynamical vertex approximation, and determinant quantum Monte Carlo. In contrast to the archetypal square lattice, we find no tendencies toward magnetic ordering, as magnetic correlations remain short-range. Nevertheless, the magnetic correlations undergo a remarkable crossover as the system approaches the metal-to-insulator transition. The Mott transition itself does not affect the magnetic correlations. Our equal-time and dynamical structure factors can be used as a reference for inelastic neutron scattering experiments on the growing family of metallic kagome materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Low-stress creep behavior of multiple salt caverns under cyclic operations

Here, the use of multiple salt caverns for large-scale underground hydrogen storage offers a strategic solution to the growing demand for efficient and flexible energy storage, due to the inherent low permeability, high mechanical strength, and self-healing properties of the salt formation. Despite these advantages, the long-term geomechanical response of salt caverns under cyclic injection and withdrawal remains a significant challenge for ensuring operational stability. This mechanistic study highlights the critical role of low-stress creep, also known as pressure solution creep, in governing deformation of salt caverns during cyclic operations. Unlike conventional creep mechanisms that dominate under high-stress conditions, low-stress creep becomes particularly relevant under the moderate stress changes induced by repeated injection and withdrawal, which provides a previously underexplored control on cavern closure. Our three-dimensional computational model integrates the low-stress creep mechanism into the Munson–Dawson creep equation across a spectrum of operational scenarios including variations in cavern pressure cycles, injection-withdrawal frequencies, and caprock mechanical property. The low-stress creep components accelerate the cavern creep closure, which is amplified with shorter cycle frequency and larger pressure difference. Sensitivity analyses capture the complex interactions between multiple caverns and surround formations at the field scale that allows for a quantitative assessment of deformation patterns and closure rates over time and thereby informs the design and operation of sustainable underground hydrogen storage system.

Cyclic operation↗

Online data-driven changepoint detection for high-dimensional dynamical systems

In this study, the detection of anomalies or transitions in complex dynamical systems is of critical importance to various applications. In this study, we propose the use of machine learning to detect changepoints for high-dimensional dynamical systems. Here, changepoints indicate instances in time when the underlying dynamical system has a fundamentally different characteristic—which may be due to a change in the model parameters or due to intermittent phenomena arising from the same model. We propose two complementary approaches to achieve this, with the first devised using arguments from probabilistic unsupervised learning and the latter devised using supervised deep learning. To accelerate the deployment of transition detection algorithms in high-dimensional dynamical systems, we introduce dimensionality reduction techniques. Our experiments demonstrate that transitions can be detected efficiently, in real-time, for the two-dimensional forced Kolmogorov flow and the Rössler dynamical system, which are characterized by anomalous regimes in phase space where dynamics are perturbed off the attractor at potentially uneven intervals. Finally, we also demonstrate how variations in the frequency of detected changepoints may be utilized to detect a significant modification to the underlying model parameters by utilizing the Lorenz-63 dynamical system.

97 MATHEMATICS AND COMPUTING↗

Material properties and mechanical behaviour of functionally graded steel produced by wire-arc additive manufacturing

Metal Big Area Additive Manufacturing is an additive manufacturing technique based on Gas Metal Arc Welding (GMAW) with the option to use many shielding gases, and materials. The system is equipped with a dual torch design allowing for printing different materials; in our study, AISI 410 stainless steel and AWS ER70S-6 mild steel are both printed in the same component. Different print strategies were designed to highlight changes in material and mechanical properties. Deformation behaviour of a materials’ interface was analysed by two-dimensional digital image correlation of uniaxial tensile specimens in displacement-controlled tests. Instances of non-homogeneous local strains adjacent to the interface are observed, as well as variability in mechanical behaviour and microstructure based on location within the print. Optical and electron microscopy are used to evaluate three microstructural zones in a 5 mm range of the interface between mild steel and stainless steel. Areas far from the interface produced polygonal ferrite and pearlite, while areas close to the interface produced acicular ferrite and bainite. Chromium redistribution profiles are dependent on the print strategy used, as shown by scanning electron microscopy with Energy dispersive spectroscopy. Evidence produced via electron backscatter diffraction is shown to support the argument that transformation induced plasticity is not the cause for the non-homogeneous deformation.

36 MATERIALS SCIENCE↗

Advanced strategies for the development of porous carbon as a Li host/current collector for lithium metal batteries

Lithium metal is considered a promising anode material for high-energy-density rechargeable batteries because of its high specific theoretical capacity (3860 mAh g -1 , low mass density (0.534 g cm -3 ), and low electrochemical redox potential (-3.04 V vs. the standard hydrogen electrode). However, the high reactivity of Li with the electrolyte leads to the formation of an unstable solid electrolyte interphase (SEI) and continuous side reactions. Also, the non-uniform lithium-ion flux and infinite volume expansion of Li metal cause the growth of Li dendrites. These pose significant safety challenges and cause rapid capacity fading of the lithium metal batteries (LiMBs). To resolve these issues, a low-cost, easily processed, lightweight, high-performance carbon-based porous matrix is considered promising to host Li metal deposition. The three-dimensional (3D) porous nano/microstructured carbon provides sufficient space for Li accommodation during Li plating, buffers the volume changes during Li plating/stripping, and lowers the effective current density contributing to dendrite-free Li deposition. Besides, the outstanding electrochemical and mechanical stability, flexibility and the high electronic conductivity enable the nano/microstructured carbon to serve as both Li host and current collector. The development of 3D carbon/Li composite by mechanical roll-press techniques not only eliminates the complex and risky procedure of making carbon/Li composite based on Li plating or molten Li infusion but also stabilizes the capacity at higher Li plating/stripping rates. Recently, there is an advancement in the lithiophilic decorations of 3D structure to introduce sufficient nucleation sites and the development of artificial SEI on top of the 3D matrix to suppress Li dendrite formation. Such 3D structural modifications create a uniform electric field, lower the Li nucleation overpotential, provide strong mechanical and chemical stability, and stabilize the interface thereby inhibiting the degradation of lithium and the electrolyte. Here we summarize the research progress on porous carbon/Li composites in terms of materials type, structure, fabrication technique, their electrochemical battery performance, and identify the critical challenges that need to be addressed for high-energy-density practical LiMBs.

25 ENERGY STORAGE↗

Tracking of Marangoni driven motion during laser powder bed fusion

Laser Powder Bed Fusion (LPBF) can be used to create Functionally Graded Materials (FGMs) by selectively distributing property augmenting particles throughout the build matrix. With this method parts can be created with nonhomogeneous properties tuned to spatially varied, pre-determined design constraints. To unlock this capability, the fluid motion that occurs in the molten liquid phase must be thoroughly understood. More importantly, the actual tracking of motion during the LPBF process is needed. Further, a numerical model of heat transfer and fluid flow in LPBF process was created. Using results from the model the motion of particles starting at many different locations was tracked. The average change in position for these particles based on starting location was calculated. The effects of non-dimensional parameters on melt pool size were examined. These results were validated experimentally and compared to what is available in the literature.

42 ENGINEERING↗

LoTToR: An Algorithm for Missing-Wedge Correction of the Low-Tilt Tomographic 3D Reconstruction of a Single-Molecule Structure

A single-molecule three-dimensional (3D) structure is essential for understanding the thermal vibrations and dynamics as well as the conformational changes during the chemical reaction of macromolecules. Individual-particle electron tomography (IPET) is an approach for obtaining a snap-shot 3D structure of an individual macromolecule particle by aligning the tilt series of electron tomographic (ET) images of a targeted particle through a focused iterative 3D reconstruction method. The method can reduce the influence on the 3D reconstruction from large-scale image distortion and deformation. Due to the mechanical tilt limitation, 3D reconstruction often contains missing-wedge artifacts, presented as elongation and an anisotropic resolution. Here, we report a post-processing method to correct the missing-wedge artifact. This low-tilt tomographic reconstruction (LoTToR) method contains a model-free iteration process under a set of constraints in real and reciprocal spaces. A proof of concept is conducted by using the LoTToR on a phantom, i.e., a simulated 3D reconstruction from a low-tilt series of images, including that within a tilt range of ±15°. The method is validated by using both negative-staining (NS) and cryo-electron tomography (cryo-ET) experimental data. A significantly reduced missing-wedge artifact verifies the capability of LoTToR, suggesting a new tool to support the future study of macromolecular dynamics, fluctuation and chemical activity from the viewpoint of single-molecule 3D structure determination.

97 MATHEMATICS AND COMPUTING↗

Quantitative metrics for evaluating thermonuclear design codes and physics models applied to the National Ignition Campaign

In this study, physics models and design codes for hot dense plasmas undergoing thermonuclear burn are evaluated objectively using statistical metrics that compare the difference between calculations and data relative to the experimental uncertainties. The analysis is applied to the National Ignition Campaign (NIC) because it is relevant, comprehensive, and well documented. The statistics confirm that a key process afflicting NIC performance is mix driven by hydrodynamic instabilities as approximated here using the KL model [G. Dimonte and R. Tipton, Phys. Fluids 18, 085101 (2006)]. New physics models are also presented for instability-driven magnetic fields [B. Srinivasan et al., Phys. Rev. Lett. 108, 165002 (2012)] and the Coulomb logarithm for electron–ion thermal relaxation [G. Dimonte and J. Daligault, Phys. Rev. Lett. 101, 135001 (2008)]. The plasma-generated magnetic fields improve the agreement between code and data in a statistically significant manner by reducing the electron thermal conduction in the hot-spot via the Hall term. The Coulomb logarithm is presented in a numerically practical form that incorporates recent theoretical advances. However, it does not improve the agreement between the code and data because the thermal relaxation is so fast in non-ignited NIC plasmas that the typical 20% error does not change the tight coupling between electrons and ions. Even with these improved physics models, the one-dimensional simulations presented here are not able to describe the high-convergence NIC implosions in a statistically acceptable manner. Of the heroic multi-dimensional simulations of Clark et al. [Phys. Plasmas 23, 056302 (2016)], only those in three-dimensions satisfy the statistical acceptance criterion.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Alignment of the magnetic field in star-forming regions and why it might be difficult to observe

ABSTRACT Magnetic fields are an important component of the interstellar medium (ISM) and exhibit strongly varying field strengths and a non-trivial correlation with the gas density. Its dynamical impact varies between individual regions of the ISM and correlates with the orientation of the field with respect to the gas structures. Using high-resolution magneto-hydrodynamical simulations of the ISM, we explore the connection between the orientation of the field and the dynamical state of the gas. We find that the onset of gravitational instability in molecular gas above a density of $\rho \sim 10^{-21}\, \mathrm{g\, cm}^{-3}$$(n\sim 400\, \mathrm{cm}^{-3})$ coincides with an alignment of the magnetic field lines and the gas flow. At this transition, the gradient of the density changes from mainly perpendicular to preferentially parallel to the field lines. A connection between the three-dimensional alignment and projected two-dimensional observables is non-trivial, because of a large dispersion of the magnetic field orientation along the line of sight. The turbulent correlation lengths can be small compared to the typical integration lengths. As a consequence, the small-scale signal of the orientation can sensitively depend on the line of sight or the dynamical state of the cloud can fluctuate stochastically or be completely averaged out. With higher spatial resolution more small-scale structures are resolved, which aggravates the link between magneto-hydrodynamical quantities and projected observables.

Girichidis, Philipp (ORCID:0000000293009914)↗

Noncollinear antiferromagnetic order in the buckled honeycomb lattice of magnetoelectric Co 4 Ta 2 O 9 determined by single-crystal neutron diffraction

Co 4 Ta 2 O 9 exhibits a three-dimensional magnetic lattice based on the buckled honeycomb motif. It shows unusual magnetoelectric effects, including the sign change and nonlinearity. These effects cannot be understood without the detailed knowledge of the magnetic structure. Herein, we report neutron diffraction and direction-dependent magnetic susceptibility measurements on Co 4 Ta 2 O 9 single crystals. In this work, below 20.3 K, we find a long-range antiferromagnetic order in the alternating buckled and flat honeycomb layers of Co 2+ ions stacked along the c axis. Within experimental accuracy, the magnetic moments lie in the ab plane. They form a canted antiferromagnetic structure with a tilt angle of ~14° at 15 K in the buckled layers, while the magnetic moments in each flat layer are collinear. This is directly evidenced by a finite (0, 0, 3) magnetic Bragg peak intensity, which would be absent in the collinear magnetic order. The magnetic space group is C2/c'. It is different from the previously reported C2/c' group, also found in the isostructural Co 4 Nb 2 O 9 . The revised magnetic structure successfully explains the major features of the magnetoelectric tensor of Co 4 Ta 2 O 9 within the framework of the spin-flop model.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measuring the properties of f - mode oscillations of a protoneutron star by third-generation gravitational-wave detectors

Core-collapse supernovae are among the astrophysical sources of gravitational waves that could be detected by third-generation gravitational-wave detectors. Here, we analyze the gravitational-wave strain signals from two- and three-dimensional simulations of core-collapse supernovae generated using the code FORNAX. A subset of the two-dimensional simulations has non-zero core rotation at the core bounce. A dominant source of time changing quadrupole moment is the l = 2 fundamental mode (f- mode) oscillation of the proto-neutron star. From the time-frequency spectrogram of the gravitational-wave strain we see that, starting ~ 400 ms after the core bounce, most of the power lies within a narrow track that represents the frequency evolution of the f-mode oscillations. The f-mode frequencies obtained from linear perturbation analysis of the angle averaged profile of the protoneutron star corroborate what we observe in the spectrograms of the gravitational wave signal. We explore the measurability of the f-mode frequency evolution of protoneutron star for a supernova signal observed in the third-generation gravitational-wave detectors. Measurement of the frequency evolution can reveal information about the masses, radii, and densities of the proto-neutron stars. We find that if the third generation detectors observe a supernova within 10 kpc, we can measure these frequencies to within ~90% accuracy. Here, we can also measure the energy emitted in the fundamental f-mode using the spectrogram data of the strain signal. We find that the energy in the f-mode can be measured to within 20% error for signals observed by Cosmic Explorer using simulations with successful explosion, assuming source distances within 10 kpc.

79 ASTRONOMY AND ASTROPHYSICS↗

Quantification of Energy Savings and Demand Reduction for a Heat Pump Integrated with Thermal Energy Storage (Final Report)

To mitigate the variation in demand on the electric grid, thermal energy storage (TES) is an alternative to electric batteries or installing new peaking power plants. Stakeholders and policy makers across the United States have expressed interests in promoting TES, as demonstrated by the US Department of Energy’s Grid-Interactive Efficient Buildings program and the efforts of various state legislatures. However, the cost value provided by TES are unclear. If reliable cost benefits were determined, stakeholders would have a clearer picture of the financial returns that can be gained from their investment in TES. The study in this report is conducted by ORNL with collaboration with Emerson the Helix Innovation Center. In the first part of this report, EnergyPlus was used to perform whole-building simulations for two residential buildings in Indianapolis and Atlanta. The HVAC system in both buildings were equipped with phase change material TES. The TES tank was charged in off-peak hours and discharged in peak hours to perform load shifting. First, the economic value implied by existing time-of-use (TOU) rates offered by utility companies was analyzed via whole-building simulation. Second, existing demand reduction (DR) incentives sourced from 3 different electrical grid administrators (i.e., California, Texas, and New England region) were surveyed to determine their implied value. The study suggests that the traditional value analysis that focuses on ROI for the building owner significantly undervalues TES technology making economic viability difficult. A more comprehensive value analysis that includes peak demand management and deferred capital for peaking power plants shows that TES should be economically viable but here the value is greater for the utility and requires large market penetration and aggregation to fully realize the benefits. Therefore, to facilitate commercialization, new business models are needed that include a broader range of stakeholders and distribute the value of TES proportionally. In the 2 nd part of this project, the benefits of a novel phase change material (PCM) integrated heat pump configuration were evaluated via detailed component based simulation. A one-dimensional PCM heat exchanger model which discretizes the PCM tank and refrigerant tubes into small control volumes is developed. Each control volume can have different PCM temperatures, PCM properties, and heat transfer coefficients. The PCM tank is charged by a wrapped tank condenser and discharged by an internal refrigerant coil. The PCM heat exchanger model is integrated into DOE/ORNL Heat Pump Design Model for heat pump system simulation. To demonstrate the performance of the PCM integrated heat pump, a case study in Chicago was performed. A Time-of-Use utility structure-based control strategy is implemented to schedule the PCM tank charging and discharging mode switching. Compared with a conventional electric heat pump, the PCM integrated heat pump shows superior performance on load shifting and utility cost reduction. As a result, the proposed system demonstrates 24.6% utility saving for cooling application and 25.8% utility saving for heating application.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Signatures of aerosol-cloud interactions in GiOcean: a coupled global reanalysis with two-moment cloud microphysics

Aerosols influence the Earth's radiative balance through direct interactions with radiation and by affecting cloud properties. Anthropogenic aerosols have led to cooling during the industrial era through aerosol–cloud interactions (ACI), including aerosol effects on cloud microphysical properties and the subsequent adjustments. However, large uncertainties remain in Earth system models (ESMs) regarding the magnitude of this cooling. In part, ESMs substantially disagree on cloud properties, thermodynamics, the hydrological cycle, and general circulation. Reanalysis provides a useful avenue for exploring the impact of ACI on clouds and radiation because its atmosphere is forced to match realistic conditions through the assimilation of observations. Here, we explore the impact of ACI on clouds in the GiOcean reanalysis – the first to incorporate aerosol-cloud interactions. We contrast variables important for ACI between GiOcean and satellite observations and develop 2-dimensional lookup tables of ACI for both using a source-sink budget perspective to attribute the changes in cloud droplet number (Nd) and liquid water path (LWP) to aerosol and meteorology. A compositing analysis using lookup tables shows that GiOcean captures key aspects of aerosol–cloud–precipitation interactions, including (1) activation of aerosol into cloud droplets, (2) effective precipitation scavenging of Nd, (3) suppression of precipitation by high Nd in regions with heavy aerosol emissions. In contrast, satellite observations do not exhibit clear patterns for processes (2) and (3). Random Forest analysis shows that interannual variability in Nd and LWP over the Northern Hemisphere ocean in GiOcean is primarily driven by precipitation, consistent with satellite observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Surface pressure measurements on the blade of an operating Mod-2 wind turbine with and without vortex generators

Pressure measurements covering a range of wind velocities were made at one span location on the surface of an operating Mod-2, 2500 kW, wind turbine blade. The data, which were taken with and without vortex generators installed on the leading edge, show the existence of higher pressure coefficients than would be expected from two-dimensional wind tunnel data. These high pressure ratios may be the result of three-dimensional flow over the blade, which delays flow separation. Data are presented showing the repetitiveness of abrupt changes in the pressure distribution that occur as the blade rotates. Calculated values of suction and flap coefficients are also presented.

Nyland, Ted W.↗

Chordwise pressure measurements on a blade of Mod-2 Wind Turbine

Pressure measurements covering a range of wind velocities were made at one span location on a blade of the Mod-2 Wind Turbine. The data show the existence of higher pressure coefficients than would be expected from wind tunnel data. These high pressure coefficients may be the result of three-dimensional flow over the blade that delays flow separations. Data is presented showing the repetitiveness and abrupt changes in the pressure distribution that occurs as the blade rotates. Calculated values of suction and flap coefficients are also presented.

Nyland, T. W.↗