Mapping renormalized coupled cluster methods to quantum computers through a compact unitary representation of nonunitary operators
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97 MATHEMATICS AND COMPUTING↗
SEARCH · Engineering Papers
Results for “electronic structure method”
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Use of Transmission Electron Microscopy for Analysis of Aerosol Particles and Strategies for Imaging Fragile Particles
For over 25 years, transmission electron microscopy (TEM) has provided a method for the study of aerosol particles with sizes from below the optical diffraction limit to several microns, resolving the particles as well as smaller features. The wide use of this technique to study aerosol particles has contributed important insights about environmental aerosol particle samples and model atmospheric systems. TEM produces an image that is a 2D projection of aerosol particles that have been impacted onto grids and, through associated techniques and spectroscopies, can contribute additional information such as the determination of elemental composition, crystal structure, and 3D particle structures. Soot, mineral dust, and organic/inorganic particles have all been analyzed using TEM and spectroscopic techniques. TEM, however, has limitations that are important to understand when interpreting data including the ability of the electron beam to damage and thereby change the structure and shape of particles, especially in the case of particles composed of organic compounds and salts. In this paper, we concentrate on the breadth of studies that have used TEM as the primary analysis technique. Another focus is on common issues with TEM and cryogenic-TEM. Insights for new users on best practices for fragile particles, that is, particles that are easily susceptible to damage from the electron beam, with this technique are discussed. Tips for readers on interpreting and evaluating the quality and accuracy of TEM data in the literature are also provided and explained.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Computational Evaluation of Thermal Response of Open-Cell Foam With Circular Pore (Computional Evaluation of Thermal Response of Open-Cell Foam with Circular Pore)
The evaluation of effective material properties in heterogeneous materials (e.g., composites or multicomponent structures) critically relevant to a wide spectrum of applications, including nuclear power, electronic packaging, flame retardants, hypersonics, and gas turbine power. The work described in this paper is centered around the numerical assessment of the thermal behavior of porous materials obtained from finite element thermal modeling and simulation. Here, two-dimensional, steady state analyses were performed on unit cells with centered, circular pores using a second order accurate Galerkin finite element method (FEM). The effective thermal conductivities of the porous systems were examined, encompassing a range of porosities from 4.9% to 60.1%. The geometries of the models were generated based on ordered circular pores for each modeled porosity level. The system response quantity (SRQ) under investigation was the dimensionless effective thermal conductivity across the unit cell. The dimensionless effective thermal conductivity was compared across all simulated cases, producing a trend between porosity and effective thermal conductivity. In the presented investigation, the method of manufactured solutions (MMS) was used to perform code verification, and the grid convergence index (GCI) was employed to estimate discretization uncertainty as solution verification. Code verification concluded an approximately second order accurate Galerkin FEM solver. It was found that the introduction of porosity to the unit cell material structure reduces effective thermal conductivity, as anticipated. Numerical results obtained in this study are compared to an analytical solution and to a sample of empirical data.
36 MATERIALS SCIENCE↗
Cactus-like NiCo 2 S 4 @NiFe LDH hollow spheres as an effective oxygen bifunctional electrocatalyst in alkaline solution
The high-performance non-precious electrocatalysts for both oxygen redn. reaction (ORR) and oxygen evolution reaction (OER) are crucial to the practical application of fuel cells and metal-air batteries. Herein, a novel cactus-like NiCo 2 S 4 @NiFe LDH hollow sphere assembled by one-dimensional (1D) NiFe LDH nanowires and two-dimensional (2D) NiFe LDH nanosheets on the NiCo 2 S 4 hollow spheres is prepd. by a facile hydrothermal method. The outer NiFe LDH nanowires and NiFe LDH nanosheets can effectively suppress the collapse and corrosion of inner NiCo 2 S 4 hollow structure during long-term stability tests. The integration of the effective OER electrocatalyst NiFe LDH into NiCo 2 S 4 to form heterostructures, as well as the strong electronic interaction between NiCo 2 S 4 and NiFe LDH, can greatly boost both ORR and OER activities. Due to the above merits, the NiCo 2 S 4 @NiFe LDH achieves remarkably a small potential gap (ΔE = E j =10-E 1/2 ) of only 0.667 V. In this paper, we offer a facile strategy to design efficient catalysts with heterostructures.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Bayesian optimization of entropy-stabilized metal fluoride conversion cathodes and their synthesis
Fluoride-based conversion cathodes are promising for next-generation Li ion batteries because of their high voltage and energy densities. High entropy earth abundant fluoride cathodes are attractive for sustainable battery because of the potentially higher cycling stability. While Ni and Co containing equimolar alloys stabilized by high entropy were considered previously, Ni and Co free non-equimolar metal alloy compositions might offer new opportunities to increase materials stability and average voltage. This opportunity was pursued using Bayesian optimization of average voltage for the computational prediction of (Fe x1 Cu x2 Zn x3 Mn x4 Mg x5 )F 2 cathode chemistries. Theoretical voltage, room temperature free energy, and electronic structure of potentially high voltage compositions were computed using density functional theory calculations. Here, the experimental realization of non-equimolar quinary Co and Ni free fluorides with stable rutile single phase and improved conversion reaction voltage by up to 28 % compared to the equimolar alloy demonstrated the power of Bayesian optimization methods for the computationally guided experimental synthesis of fluoride cathodes. Finally, non-equimolar cathode chemistries were found with cycling stability superior to known multi-element fluorides.
25 ENERGY STORAGE↗
Absolute nuclear charge radius by Na-like spectral line separation in high-Z elements
Abstract We describe a novel technique to determine absolute nuclear radii of high- Z nuclides. Utilizing accurate theoretical atomic structure calculations together with precise measurements of extreme ultraviolet transitions in highly charged ions this method allows for precise determinations of absolute nuclear charge radii based upon the well-known nuclear radii of their neighboring elements. This method can work for elements without stable isotopes, and its accuracy may be competitive with current methods (electron scattering and muonic x-ray spectroscopy).
Hosier, A. (ORCID:0000000328366605)↗
Microstructural and Superconducting Radiofrequency Properties of Multilayer Sequentially Sputtered Nb 3 Sn films
Nb 3 Sn is considered as a potential candidate for superconducting radiofrequency cavities for particle acceleration due to its higher transition temperature of 18.3 K and higher superheating field of 400 mT. Nb 3 Sn films can be grown inside the surface of a Nb cavity by sequentially sputtering multiple layers of Nb and Sn thin films followed by annealing at 950 °C for 3 h. We report on the properties of Nb 3 Sn films grown on Nb substrates by magnetron sputtering. The films’ crystal structure, surface morphology, and composition were characterized by X-ray diffraction, scanning electron microscopy, and energy-dispersive X-ray spectroscopy. The films had a polycrystalline Nb 3 Sn structure with a fine-grain surface and an atomic Sn composition of ~23%. The RF surface resistance of the films was measured for different temperatures at 7.4 GHz to understand the feasibility of this method for the SRF application. The RF surface resistance of the films was 5 mΩ at 12 K, which is about 2 orders of magnitude higher than 60 μΩ previously measured in Nb 3 Sn films grown by Sn vapor diffusion. Finally, the sputtered film had a superconducting transition at 17.2 K, which is also lower than 17.9 K observed in Nb 3 Sn film prepared by vapor diffusion.
43 PARTICLE ACCELERATORS↗
Improving high temperature resilience of fiber sensor embedded smart components through laser shock peening
This study explores the use of laser shock peening (LSP) to enhance material properties and high-temperature performance of fiber-sensor-fused smart parts fabricated by additive manufacturing (AM) methods. Using embedded fiber sensors as distributed strain gauges, the study demonstrates that LSP can induce compressive strains of up to 130 µε on fiber embedded 1-mm below metal surfaces. The electron backscatter diffraction (EBSD) analysis shows that, with optimized LSP parameters, the metallic matrix undergoes substantial microstructural refinement, resulting in denser structures. Thermal cycling tests showed that the LSP process can increase fiber slippage temperatures by more than 50 °C. This work shows that the LSP process is an effective room-temperature process for enhancing both surface quality and increasing fiber slippage threshold under both thermal and mechanical stress.
Zhong, Shuda [University of Pittsburgh, PA (United↗
The crystal structure of feitknechtite (β-MnOOH) and a new MnOOH polymorph
Studies suggest that feitknechtite (β-MnOOH) is a prevalent, and perhaps necessary, intermediate phase during the synthesis of birnessite-like phases, the abiotic oxidation of Mn2+, and the transformation of biogenic hexagonal phyllomanganates to more complex Mn oxides in laboratory and natural systems. Researchers have generally described feitknechtite as consisting of pyrochroite-like (or cadmium iodide-like) Mn-O octahedral layers, but a detailed crystal structure has not been reported. For this work, we used TEM/SAED and powder XRD and Rietveld refinements to derive the unit cell and, for the first time, report a complete structure description for feitknechtite (β-MnOOH). Rietveld refinements were also completed for three natural feitknechtite/hausmannite samples, and time-resolved synchrotron XRD experiments were used to follow the thermal transformation of feitknechtite to hausmannite. Additionally, we identified and report the structure for a second, and perhaps novel, MnOOH polymorph (proposed designation ε-MnOOH), mixed with the synthetic feitknechtite, that is similar to β-MnOOH but with a different layer stacking.
58 GEOSCIENCES↗
Plasma heating technology
The operational environment for plasma heating systems presents unprecedented challenges for the success of magnetic fusion. This chapter discusses the current state of ion cyclotron and electron cyclotron heating systems and the research and development priorities needed to establish working solutions for these systems. While much progress has been made, there is much more work to be done to make fusion energy commercially viable. Research and development priorities include radiation-resistant structural and plasma facing materials, advanced manufacturing methods, new cooling methods, first-wall integrated actuators, improvements in power source efficiency, higher frequency gyrotrons, and improved overall system reliability.
Caughman, John↗
Growth and characterization of homoepitaxial β-Ga 2 O 3 layers
ß-Ga 2 O 3 is a next-generation ultra-wide bandgap semiconductor (E g = 4.8 eV to 4.9 eV) that can be homoepitaxially grown on commercial substrates, enabling next-generation power electronic devices among other important applications. Analyzing the quality of deposited homoepitaxial layers used in such devices is challenging, in part due to the large probing depth in traditional x-ray diffraction (XRD) and also due to the surface-sensitive nature of atomic force microscopy (AFM). Here, a combination of evanescent grazing-incidence skew asymmetric XRD and AFM are investigated as an approach to effectively characterize the quality of homoepitaxial ß-Ga 2 O 3 layers grown by molecular beam epitaxy at a variety of Ga/O flux ratios. Accounting for both structure and morphology, optimal films are achieved at a Ga/O ratio of ~1.15, a conclusion that would not be possible to achieve by either XRD or AFM methods alone. Finally, fabricated Schottky barrier diodes with thicker homoepitaxial layers are characterized by J-V and C-V measurements, revealing an unintentional doping density of 4.3×10 16 cm -3 - 2×10 17 cm -3 in the epilayer. These results demonstrate the importance of complementary measurement methods for improving the quality of the ß-Ga 2 O 3 homoepitaxial layers used in power electronic and other devices.
36 MATERIALS SCIENCE↗
Origin of the ring ellipticity in the black hole images of M87*
We investigate the origin of the elliptical ring structure observed in the images of the supermassive black hole M87*, aiming to disentangle contributions from gravitational, astrophysical, and imaging effects. Leveraging the enhanced capabilities of the Event Horizon Telescope (EHT)'s 2018 array, including improved (u,v)-coverage from the Greenland Telescope, we measured the ring's ellipticity using five independent imaging methods, obtaining a consistent average value of τ = 0.08−0.02+0.03 with a position angle of ξ = 50.1−7.6+6.2 degrees. To interpret this measurement, we compared it to general relativistic magnetohydrodynamic (GRMHD) simulations spanning a wide range of physical parameters including the thermal or nonthermal electron distribution function, spins, and ion-to-electron temperature ratios in both low- and high-density regions. We find no statistically significant correlation between spin and ellipticity in GRMHD images. Instead, we identify a correlation between ellipticity and the fraction of non-ring emission, particularly in nonthermal models and models with higher jet emission. These results indicate that the ellipticity measured from the M87* emission structure is consistent with that expected from simulations of turbulent accretion flows around black holes, where it is dominated by astrophysical effects rather than gravitational ones. Future high-resolution imaging, including space very long baseline interferometry and long-term monitoring, will be essential to isolate gravitational signatures from astrophysical effects.Key words: accretion, accretion disks / black hole physics / gravitation / galaxies: active** These authors have contributed equally to this work.*** NASA Hubble Fellowship Program, Einstein Fellow.† Deceased.
Dahale, Rohan [Granada U., Theor. Phys. Astrophys.↗
Laser-Assisted Synthesis of Monolayer 2D MoSe 2 Crystals with Tunable Vacancy Concentrations: Implications for Gas and Biosensing
We report tuning the structural and electronic properties of atomically thin two-dimensional (2D) materials via defect and vacancy engineering is the key to enabling their potential use in various applications, including electronics, energy, and sensing devices. Vacancies are, for instance, becoming highly promising for the enhanced interaction of gases and biomolecules with 2D materials in energy and sensing applications. However, the deterministic generation of desirable vacancies with tunable concentrations remains a challenge in 2D materials due to the limitations in the current growth methods, such as the complex reaction chemistries and gas flow dynamics. Therefore, engineering defects and vacancies in 2D materials have been mainly limited to destructive top-down processes such as heating, ion bombardments, and laser postprocessing. Here, we introduce a single-step bottom-up synthesis approach for the growth of monolayer MoSe 2 crystals with tunable vacancy concentrations. This method utilizes the spatiotemporal properties and adjustable power densities of the lasers to control the vaporization dynamics of the stoichiometric MoSe 2 powders. Such a mechanism in the vaporization allows us to grow tunable stoichiometry monolayer MoSe 2–x crystals on the substrates. The localized and time-controlled (250 ms to 2 s) vaporization of the MoSe 2 powder by a CO 2 laser enables the formation of monolayer crystals with controlled vacancy concentrations ranging from ~1 to 20%. The effects of laser power, laser irradiation time, and background pressure on the tuning range and subsequent properties of the crystals are investigated and quantified using Raman and photoluminescence spectroscopy, scanning transmission electron microscopy (STEM), and time-correlated single-photon counting (TCSPC). This bottom-up synthesis is a promising approach that allows the deterministic vacancy tuning for future electronics and, in particular, gas and biosensing applications without the need for further postprocessing and potential structural disruption of the crystals.
2D materials↗
Quantum sensing effect of electron tunneling in DQD/analyte complex
We investigate electron tunneling between quantum dots and molecules to propose a quantum sensor. This sensor consists of double quantum dots (DQD) with energy levels specifically tailored to mirror those of the target analyte. By analyzing the spectral distribution of electron localizations in the DQD system, we can delineate the analyte’s spectrum and deduce its composition by comparing it with a reference sample. To understand electron tunneling dynamics within the DQD/analyte complex, we performed three-dimensional computational modeling applying the effective potential approach to the InAs/GaAs heterostructure. In this modeling, we mimicked the analyte spectrum by utilizing a quantum well characterized by a quasi-discrete spectrum. Our calculations reveal the inherent potential of utilizing this method as a highly sensitive and selective sensor.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Leveraging Nitrogen Linkages in the Formation of a Porous Thorium–Organic Nanotube Suitable for Iodine Capture
We report the synthesis, characterization, and iodine capture application of a novel thorium–organic nanotube, TSN-626, [Th 6 O 4 (OH) 4 (C 6 H 4 NO 2 ) 7 (CHO 2 ) 5 (H 2 O) 3 ]·3H 2 O. The classification as a metal–organic nanotube (MONT) distinguishes it as a rare and reduced dimensionality subset of metal–organic frameworks (MOFs); the structure is additionally hallmarked by low node connectivity. TSN-626 is composed of hexameric thorium secondary building units and mixed O/N-donor isonicotinate ligands that demonstrate selective ditopicity, yielding both terminating and bridging moieties. Because hard Lewis acid tetravalent metals have a propensity to bind with electron donors of rival hardness (e.g., carboxylate groups), such Th–N coordination in a MOF is uncommon. However, the formation of key structural Th–N bonds in TSN-626 cap some of the square antiprismatic metal centers, a position usually occupied by terminal water ligands. TSN-626 was characterized by using complementary analytical and computational techniques: X-ray diffraction, vibrational spectroscopy, N 2 physisorption isotherms, and density functional theory. TSN-626 satisfies design aspects for the chemisorption of iodine. The synergy between accessibility through pores, vacancies at the metal–oxo nodes, and pendent N-donor sites allowed a saturated iodine loading of 955 mg g –1 by vapor methods. Furthermore, the crystallization of TSN-626 diversifies actinide–MOF linker selection to include soft electron donors, and these Th–N linkages can be leveraged for the investigation of metal-to-ligand bonding and unconventional topological expressions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Computation of forces and stresses in solids: Towards accurate structural optimization with auxiliary-field quantum Monte Carlo
The accurate computation of forces and other energy derivatives has been a long-standing challenge for quantum Monte Carlo methods. A number of technical obstacles contribute to this challenge. We discuss how these obstacles can be removed with the auxiliary-field quantum Monte Carlo (AFQMC) approach. AFQMC is a general, high-accuracy, many-body total-energy method for molecules and solids. The implementation of back-propagation for pure estimators allows direct calculation of gradients of the energy via the Hellmann-Feynman theorem. A planewave basis with norm-conserving pseudopotentials is used for the study of periodic bulk materials. Completeness of the planewave basis minimizes the effect of so-called Pulay terms. The ionic pseudopotentials, which can be incorporated in AFQMC in exactly the same manner as in standard independent-electron methods, regulate the force and stress estimators and eliminate any potential divergence of the Monte Carlo variances. The resulting approach allows applications of full geometry optimizations in bulk materials. As a result, it also paves the way for many-body computations of the phonon spectrum in solids.
36 MATERIALS SCIENCE↗
Nonadditive Interactions Unlock Small-Particle Mobility in Binary Colloidal Monolayers
We examine the organization and dynamics of binary colloidal monolayers composed of micron-scale silica particles interspersed with smaller-diameter silica particles that serve as minority component impurities. These binary monolayers are prepared at the surface of ionic liquid droplets over a range of size ratios (σ = 0.16–0.66) and are studied with low-dose minimally perturbative scanning electron microscopy (SEM). The high resolution of SEM imaging provides direct tracking of all particle coordinates over time, enabling a complete description of the microscopic state. In these bidisperse size mixtures, particle interactions are nonadditive because interfacial pinning to the droplet surface causes the equators of differently sized particles to lie in separate planes. By varying the size ratio, we control the extent of nonadditivity in order to achieve phase behavior inaccessible to additive 2D systems. Across the range of size ratios, we tune the system from a mobile small-particle phase (σ < 0.24) to an interstitial solid (0.24 < σ < 0.33) and furthermore to a disordered glass (σ > 0.33). These distinct phase regimes are classified through measurements of hexagonal ordering of the large-particle host lattice and the lattice’s capacity for small-particle transport. Altogether, we explain these structural and dynamic trends by considering the combined influence of interparticle interactions and the colloidal packing geometry. Our measurements are reproduced in molecular dynamics simulations of 2D nonadditive disks, suggesting an efficient method for describing confined systems with reduced dimensionality representations.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Water-Oil Displacement in Shale: New Insights from a Comparative Study Integrating Imbibition Tests and Multiscale Imaging
Water-oil displacement is an important process that occurs in a shale matrix after hydraulic fracturing and in water-based enhanced oil recovery. Current understanding of this displacement process is limited because of the complicated pore structure and surface properties in shale. In this work, this process and its controlling factors are investigated through a comparative study of three shale samples that have different types of pore systems and wettability. Here, an integrated method of imbibition and multiscale imaging was applied, and a modified oleic tracer that can better represent oil flow was used in imbibition testing and micro-computed tomography (CT) imaging. Scanning electron microscope (SEM) pore characterization was then performed under high magnification with guidance from the micro-CT images showing the changes caused by oil or water imbibition. New insights were obtained on the importance of both wettability and pore size effect on oil recovery and the distribution of residual oil after water-oil displacement. Connectivity of pores with different wettability is also discussed based on 3D analysis and SEM pore characterization. Collectively, these new findings improve the understanding of the complicated process of water-oil displacement and the role of influencing factors. Important implications for improved oil recovery strategy in shale are discussed for different types of reservoir rocks. The integrated imaging and imbibition technique provides a new path for further investigation of improved oil recovery in shale.
04 OIL SHALES AND TAR SANDS↗