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DOE OSTI2020

An Artificial Z-Scheme Constructed from Dye-Sensitized Metal Oxide Nanosheets for Visible Light-Driven Overall Water Splitting

Sensitization of a wide-gap oxide semiconductor with a visible-light-absorbing dye has been studied for decades as a means of producing H 2 from water. However, efficient overall water splitting using a dye-sensitized oxide photocatalyst has remained an unmet challenge. Here in this paper we demonstrate visible-light-driven overall water splitting into H 2 and O 2 using HCa 2 Nb 3 O 10 nanosheets sensitized by a Ru(II) tris-diimine type photosensitizer, in combination with a WO 3 -based water oxidation photocatalyst and a triiodide/iodide redox couple. With the use of Pt-intercalated HCa 2 Nb 3 O 10 nanosheets further modified with amorphous Al 2 O 3 clusters as the H 2 evolution component, the dye-based turnover number and frequency for H 2 evolution reached 4580 and 1960 h –1 , respectively. The apparent quantum yield for overall water splitting using 420 nm light was 2.4%, by far the highest among dye- sensitized overall water splitting systems reported to date. The present work clearly shows that a carefully designed dye/oxide hybrid has great potential for photocatalytic H 2 production, and represents a significant leap forward in the development of solar-driven water splitting systems.

14 SOLAR ENERGY↗

DOE OSTI2025

Smooth splitting and zeros from on-shell recursion

We describe a new approach to understanding the origins of recently discovered “hidden zeros” and “smooth splitting” of tree-level amplitudes in Tr ϕ 3 , Non-Linear Sigma Model (NLSM), Yang-Mill-Scalar (YMS) and the special Galileon. Introducing a new type of linear shift in kinematic space we demonstrate that the mysterious splitting formulae follow from a simple contour integration argument in the style of on-shell recursion. The argument makes use of only standard notions of tree-level factorization on propagators, but assumes improved UV behavior in the form of the absence of a residue at infinity. In the case of Tr ϕ 3 and NLSM this is proven by identifying our shift as a special case of a more general construction called a g-vector shift; in the case of YMS it remains an unproven conjecture. This recursive perspective leads to numerous new results: we derive generalizations of the splitting formulae on more relaxed near-zero kinematics, including interesting new kinematic limits in which the amplitude splits into a triple-product; we also demonstrate that the uncolored special Galileon model has improved UV scaling and hence also splits. We also investigate the possible realization of hidden zeros in four dimensions. The conditions under which the dimensionality constraints are compatible with zero kinematics is investigated in detail for Tr ϕ 3 and YMS; for the latter we find they can be realized only with certain restrictions on external helicity states. The realizable 4d zeros are proven by a similar recursive argument based on BCFW and is found to generalize to a new class of intrinsically 4d “helicity zeros” present in all sectors of YM and also gravity.

effective field theories↗

DOE OSTI2025

All-order splits and multi-soft limits for particle and string amplitudes

The most important aspects of scattering amplitudes have long been thought to be associated with their poles. But recently a very different sort of “split” factorizations for a wide range of particle and string tree amplitudes have been discovered away from poles. In this paper, we give a simple, conceptual origin for these splits arising from natural properties of the binary geometry of the curve integral formulation for scattering amplitudes for Tr(Φ 3 ) theory. The most natural way of “joining” smaller surfaces to build larger ones directly produces a choice of kinematics for which higher amplitudes factor into lower ones. This gives a generalization of splits to all orders in the topological expansion. These splits allow us to access and compute loop-integrated multi-soft limits for particle and string amplitudes, at all loop orders. This includes split factorizations and multisoft limits for pion and gluon amplitudes, that are related to Tr(Φ 3 ) theory by a simple kinematical shift.

Bosonic Strings↗

DOE OSTI2021

A unified formulation of splitting-based implicit time integration schemes

Splitting-based time integration approaches such as fractional step, alternating direction implicit, operator splitting, and locally one dimensional methods partition the system of interest into components, and solve individual components implicitly in a cost-effective way. Here this work proposes a unified formulation of splitting time integration schemes in the framework of general-structure additive Runge–Kutta (GARK) methods. Specifically, we develop implicit-implicit (IMIM) GARK schemes, provide the order conditions for this class, and explain their application to partitioned systems of ordinary differential equations. We show that classical splitting methods belong to the IMIM GARK family, and therefore can be studied in this unified framework. New IMIM-GARK splitting methods are developed and tested using parabolic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Electronic structure, magnetic properties, and exchange splitting of gadolinium intermetallics

Here, we report here the electronic structure calculations of the magnetic moment, magneto-crystalline anisotropy energy (MAE), and density of states (DOS) of Gd-metal, GdAl 2 , GdAl 3 , GdCo 2 , GdCo 3 , and GdCo 5 . From the DOS, the exchange splitting energy is derived to map ferrimagnetic to paramagnetic phase transition (Curie temperature, T C ). The employed theoretical method here is based on advanced density functional theory, specifically the linearized augmented plane wave method (LAPW) within the local spin density approximation (LSDA), including spin–orbit coupling (SOC) and Hubbard model parameter (U). DOS analysis of both Gd-Al and Gd-Co systems reveals a strong correlation between exchange splitting energy and T C . The Gd-Co system exhibits an enormous exchange splitting energy among Co-3d electrons, vastly overwhelming the vanishing Gd 5d exchange splitting. Finally, these findings suggest that exchange splitting of Co-3d electrons plays a key role in the ground state magnetism and magnetic transition temperatures in these materials.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Addressing the Stability Gap in Photoelectrochemistry: Molybdenum Disulfide Protective Catalysts for Tandem III–V Unassisted Solar Water Splitting

While photoelectrochemical (PEC) solar-to-hydrogen efficiencies have greatly improved over the past few decades, advances in PEC durability have lagged behind. Corrosion of semiconductor photoabsorbers in the aqueous conditions needed for water splitting is a major challenge that limits device stability. In addition, a precious-metal catalyst is often required to efficiently promote water splitting. In this work, we demonstrate unassisted water splitting using a nonprecious metal molybdenum disulfide nanomaterial catalytic protection layer paired with a GaInAsP/GaAs tandem device. This device was able to achieve stable unassisted water splitting for nearly 12 h, while a sibling sample with a PtRu catalyst was only stable for 2 h, highlighting the advantage of the nonprecious metal catalyst. In situ optical imaging illustrates the progression of macroscopic degradation that causes device failure. Furthermore, this work compares unassisted water splitting devices across the field in terms of the efficiency and stability, illustrating the need for improved stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Vortex splitting in two-dimensional fluids and non-neutral electron plasmas with smooth vorticity profiles

Initially, elliptical, quasi-two-dimensional (2D) fluid vortices can split into multiple pieces if the aspect ratio is sufficiently large due to the growth and saturation of perturbations known as Love modes on the vortex edge. Presented here are experiments and numerical simulations, showing that the aspect ratio threshold for vortex splitting is significantly higher for vortices with realistic, smooth edges than that predicted by a simple “vortex patch” model, where the vorticity is treated as piecewise constant inside a deformable boundary. The experiments are conducted by exploiting the E × B drift dynamics of collisionless, pure electron plasmas in a Penning–Malmberg trap, which closely model 2D vortex dynamics due to an isomorphism between the Drift–Poisson equations describing the plasmas and the Euler equations describing ideal fluids. The simulations use a particle-in-cell method to model the evolution of a set of point vortices. The aspect ratio splitting threshold ranges up to about twice as large as the vortex patch prediction and depends on the edge vorticity gradient. This is thought to be due to spatial Landau damping, which decreases the vortex aspect ratio over time and, thus, stabilizes the Love modes. Near the threshold, asymmetric splitting events are observed in which one of the split products contains much less circulation than the other. These results are relevant to a wide range of quasi-2D fluid systems, including geophysical fluids, astrophysical disks, and drift-wave eddies in tokamak plasmas.

Physics↗

DOE OSTI2021

Strong influence of nonmagnetic ligands on the momentum-dependent spin splitting in antiferromagnets

Here, recent studies show the nonrelativistic antiferromagnetic ordering could generate momentum-dependent spin splitting analogous to the Rashba effect but free from the requirement of relativistic spin-orbit coupling. Whereas the classification of such compounds can be illustrated by different spin-splitting prototypes (SSTs) from symmetry analysis and density-functional-theory calculations, the huge variation in chemical bonding and structures of these diverse compounds possibly clouds the issue of how much of the variation in spin splitting can be traced back to the symmetry-defined characteristics, rather to the underlining chemical and structural diversity. The alternative model Hamiltonian approaches do not confront the issues of chemical and structural complexity but often consider only the magnetic sublattice, dealing with the all-important effects of the nonmagnetic ligands via renormalizing the interactions between the magnetic sites. To this end, we constructed a DFT model Hamiltonian that allows us to study SSTs at constant chemistry while retaining the realistic atomic-scale structure including ligands. This is accomplished by using a single, universal magnetic skeletal lattice (Ni 2+ ions in rocksalt NiO) and designing small displacements of the nonmagnetic (oxygen) sublattice which produce, by design, the different SST magnetic symmetries. We show that (i) even similar crystal structures having very similar band structures can lead to contrasting behavior of spin splitting vs momentum, and (ii) even subtle deformations of the nonmagnetic ligand sublattice could cause a giant spin splitting in AFM-induced SST. This is a paradigm shift relative to the convention of modeling magnets without considering the nonmagnetic ligand that mediates indirect magnetic interaction (e.g., superexchange).

36 MATERIALS SCIENCE↗

DOE OSTI2020

Unconventional crystal-field splitting in noncentrosymmetric BaTiO 3 thin films

Understanding the crystal-field splitting and orbital polarization in noncentrosymmetric systems such as ferroelectric materials is fundamentally important. In this work, taking BaTiO 3 as a representative material, we investigate titanium crystal-field splitting and orbital polarization in noncentrosymmetric TiO 6 octahedra with resonant x-ray linear dichroism at the Ti L 2,3 edge. The high-quality BaTiO 3 thin films were deposited on DyScO 3 (110) single crystal substrates in a layer-by-layer way by pulsed laser deposition. The reflection high-energy electron diffraction and element specific x-ray absorption spectroscopy were performed to characterize the structural and electronic properties of the films. In sharp contrast to conventional crystal-field splitting and orbital configuration (d xz /d yz < d xy < d 3z 2 -r 2 < d x 2 -y 2 or d xy < d xz /d yz < d x 2 -y 2 < d 3z 2 -r 2 ) expected from compressive or tensile epitaxial strain, respectively, it is revealed that d xz , d yz , and d xy orbitals are nearly degenerate, whereas d 3z 2 -r 2 and d x 2 -y 2 orbitals are split with an energy gap ~100 meV in the epitaxial BaTiO 3 films. We find that the unexpected degenerate orbitals d xz /d yz /d xy result from the competition between the orbital splitting induced by epitaxial strain and that induced by polar distortions of BaTiO 3 films. Our results provide a route to manipulate orbital degree of freedom by switching electric polarization in ferroelectric materials.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Horizontal Split Table Conceptual Design for Advanced Reactor Validation

Oak Ridge National Laboratory and Lawrence Livermore National Laboratory are collaborating to develop a conceptual design for a horizontal split table for use in performing critical experiments. The goal of this design effort is to provide nuclear data testing and validation capabilities for advanced reactors such as pebble-bed high-temperature gas-cooled reactors, molten salt reactors, and heat pipe microreactor, but it could also be used for the current generation of reactors. The first concept being explored for the horizontal split table, a pebble-bed design based on the HTR-10 reactor, is described in this paper. A critical configuration corresponding to a footprint of about 4.5 m 2 was determined with SCALE/KENO-VI to fit the planned dimensions of the horizontal split table. The similarity of the pebble-bed design and the HTR-10 reactor application was assessed using SCALE/TSUNAMI, and a similarity coefficient $c_k$ of 0.9982 was obtained, proving that the concept will be useful for nuclear data validation and assimilation of pebble-bed type advanced reactors. In the proposed design, the materials with the highest $k_{eff}$ sensitivity are graphite and uranium, demonstrating that particular care must be given to carbon-related cross-section data. The effect of mechanical uncertainties between the fixed and moving tables was also assessed by calculating the reactivity change caused by vertical and horizontal gaps, as well as angular and torsion offsets between the two sides of the horizontal split table concept. The highest relative changes on the concept’s reactivity were caused by angular perturbations. The same analysis process is currently being used to create a molten salt advanced reactor type horizontal split table concept based on the Molten Salt Reactor Experiment (MSRE).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1982

Conservative supra-characteristics method for splitting the hyperbolic systems of gasdynamics for real and perfect gases

A conservative flux difference splitting is presented for the hyperbolic systems of gasdynamics. The stable robust method is suitable for wide application in a variety of schemes, explicit or implicit, iterative or direct, for marching in either time or space. The splitting is modeled on the local quasi one dimensional characteristics system for multi-dimensional flow similar to Chakravarthy's nonconservative split coefficient matrix method; but, as the result of maintaining global conservation, the method is able to capture sharp shocks correctly. The embedded characteristics formulation is cast in a primitive variable the volumetric internal energy (rather than the pressure) that is effective for treating real as well as perfect gases. Finally the relationship of the splitting to characteristics boundary conditions is discussed and the associated conservative matrix formulation for a computed blown wall boundary condition is developed as an example. The theoretical development employs and extends the notion of Roe of constructing stable upwind difference formulae by sending split simple one sided flux difference pieces to appropriate mesh sites. The developments are also believed to have the potential for aiding in the analysis of both existing and new conservative difference schemes.

Lombard, C. K.↗

NASA NTRS1991

A new flux splitting scheme

A new flux splitting scheme is proposed. The scheme is remarkably simple and yet its accuracy rivals and in some cases surpasses that of Roe's solver in the Euler and Navier-Stokes solutions performed in this study. The scheme is robust and converges as fast as the Roe splitting. An approximately defined cell-face advection Mach number is proposed using values from the two straddling cells via associated characteristic speeds. This interface Mach number is then used to determine the upwind extrapolation for the convective quantities. Accordingly, the name of the scheme is coined as Advection Upstream Splitting Method (AUSM). A new pressure splitting is introduced which is shown to behave successfully, yielding much smoother results than other existing pressure splittings. Of particular interest is the supersonic blunt body problem in which the Roe scheme gives anomalous solutions. The AUSM produces correct solutions without difficulty for a wide range of flow conditions as well as grids.

Liou, Meng-Sing↗

NASA NTRS1993

An upwind, kinetic flux-vector splitting method for flows in chemical and thermal non-equilibrium

We have developed new upwind kinetic difference schemes for flows with non-equilibrium thermodynamics and chemistry. These schemes are derived from the Boltzmann equation with the resulting Euler schemes developed as moments of the discretized Boltzmann scheme with a locally Maxwellian velocity distribution. Splitting the velocity distribution at the Boltzmann level is seen to result in a flux-split Euler scheme and is called Kinetic Flux Vector Splitting (KFVS). Extensions to flows with finite-rate chemistry and vibrational relaxation is accomplished utilizing nonequilibrium kinetic theory. Computational examples are presented comparing KFVS with the schemes of Van Leer and Roe for a quasi-one-dimensional flow through a supersonic diffuser, inviscid flow through two-dimensional inlet, and viscous flow over a cone at zero angle-of-attack. Calculations are also shown for the transonic flow over a bump in a channel and the transonic flow over an NACA 0012 airfoil. The results show that even though the KFVS scheme is a Riemann solver at the kinetic level, its behavior at the Euler level is more similar to the existing flux-vector splitting algorithms than to the flux-difference splitting scheme of Roe.

Eppard, W. M.↗

NASA NTRS1993

A new flux splitting scheme

Liou, Meng-Sing↗

NASA NTRS1996

Experimental Study of Split-Path Transmission Load Sharing

Split-path transmissions are promising, attractive alternatives to the common planetary transmissions for helicopters. The split-path design offers two parallel paths for transmitting torque from the engine to the rotor. Ideally, the transmitted torque is shared equally between the two load paths; however, because of manufacturing tolerances, the design must be sized to allow for other than equal load sharing. To study the effect of tolerances, experiments were conducted using the NASA split-path test gearbox. Two gearboxes, nominally identical except for manufacturing tolerances, were tested. The clocking angle was considered to be a design parameter and used to adjust the load sharing of an otherwise fixed design. The torque carried in each path was measured for a matrix of input torques and clocking angles. The data were used to determine the optimal value and a tolerance for the clocking angles such that the most heavily loaded split path carried no greater than 53 percent of an input shaft torque of 367 N-m. The range of clocking angles satisfying this condition was -0.0012 +/- 0.0007 rad for box 1 and -0.0023 +/- 0.0009 rad for box 2. This study indicates that split-path gearboxes can be used successfully in rotorcraft and can be manufactured with existing technology.

Krantz, Timothy L.↗

NASA NTRS2002

Multi-dimensional Upwind Fluctuation Splitting Scheme with Mesh Adaption for Hypersonic Viscous Flow

A multi-dimensional upwind fluctuation splitting scheme is developed and implemented for two-dimensional and axisymmetric formulations of the Navier-Stokes equations on unstructured meshes. Key features of the scheme are the compact stencil, full upwinding, and non-linear discretization which allow for second-order accuracy with enforced positivity. Throughout, the fluctuation splitting scheme is compared to a current state-of-the-art finite volume approach, a second-order, dual mesh upwind flux difference splitting scheme (DMFDSFV), and is shown to produce more accurate results using fewer computer resources for a wide range of test cases. A Blasius flat plate viscous validation case reveals a more accurate upsilon-velocity profile for fluctuation splitting, and the reduced artificial dissipation production is shown relative to DMFDSFV. Remarkably, the fluctuation splitting scheme shows grid converged skin friction coefficients with only five points in the boundary layer for this case. The second half of the report develops a local, compact, anisotropic unstructured mesh adaptation scheme in conjunction with the multi-dimensional upwind solver, exhibiting a characteristic alignment behavior for scalar problems. The adaptation strategy is extended to the two-dimensional and axisymmetric Navier-Stokes equations of motion through the concept of fluctuation minimization.

Wood, William A., III↗

NASA NTRS1941

Wind-Tunnel Investigation of an NACA 66,2-216 Low-Drag Wing with Split Flaps of Various Sizes, Special Report

An investigation was conducted in the NACA 19-foot pressure wind tunnel of a rectangular wing having NACA 66, 2-216 low-drag airfoil sections and various sizes of simple split flaps. The purpose of the investigation was, primarily, to determine the influence of these flap installations on the aerodynamic characteristics of the wing. Complete lift, drag, and pitching-moment characteristics were determined for a range of test Reynolds numbers from about 2,600,000 to 4,600,000 for each of the installations and for the plain wing. The results of this investigation indicate that values of maximum lift coefficient similar to those of wings with conventional airfoil sections and split flaps can be expected of wings having the NACA 66,2-216 low-drag sections. The increment of maximum lift due to the split flap was found to be practically independent of the Reynolds number over the range investigated. The optimum split flap on the basis of maximum lift appears to have a chord about 20% of the wing chord and a deflection of 60 degrees. The C(sub L) max of the wing with the 0.20c partial-span flap deflected 60 degrees is 2.07 at a Reynolds number of 4,600,000 while with the full-span flap it is approximately 2.53; the increment of the maximum lift coefficient due to the flap is approximately proportional to the flap span. Although the addition of a split flap tends to hasten the stall and to cause it to occur more abruptly, little change in pattern is evidenced by observations of the behavior of wool tufts on the wing.

Muse, Thomas C.↗

NASA NTRS1941

Wind-Tunnel Investigation of an NACA Low-Drag Tapered Wing with Straight Trailing Edge and Simple Split Flaps, Special Report

An investigation was conducted in the NACA 19-foot pressure wind tunnel of a tapered wing with straight railing edge having NACA 66 series low-drag airfoil sections and equipped with full-span and partial-span simple split flaps. The airfoil sections used were the NACA 66,2-116 at the root and the 66,2-216 at the tip. The primary purpose of the investigation was to determine the effect of the split flaps on the aerodynamic characteristics of the tapered wing. Complete lift, drag, and pitching-moment coefficients were determined for the plain wing and for each flap arrangement through a Reynold number range of 2,600,000 to 4,600,000. The results of this investigation indicate that values of maximum lift coefficient comparable to values obtained on tapered wings with conventional sections and similar flap installations can be obtained from wings with the NACA low-drag sections. The increment of maximum lift due to the split flap was found to vary somewhat with Reynold number over the range investigated. The C(sub L)max of the wing alone is 1.49 at a Reynolds number of 4,600,000; whereas with the partial-span simple split flap it is 2.22 and with the full-span arrangement, 2.80. Observations of wool tufts on the wing indicate that the addition of split flaps did not appreciable alter the pattern of the stall; even though the stall did occur more abruptly than with the wing alone.

Muse, Thomas C.↗