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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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The electron and photon reconstruction and identification algorithms used by the D0 Collaboration at the Fermilab Tevatron collider are described. The determination of the electron energy scale and resolution is presented. Studies of the performance of the electron and photon reconstruction and identification are summarized.
In this work, we report observations of an intense, multi-band, sub-THz and THz radiation extracted from a similar to 2-3 MeV electron beam with a flat transverse profile propagating in an oversized rectangular waveguide placed into a 3.25 mm gap of a planar undulator having 1.3 cm period and similar to 20 cm length. Radiation outcoupling is accomplished using a horn antenna and a miniature permanent in-vacuum magnet separating the mm-sub-mm-waves and electron beam. A table-top experiment utilizes a radio frequency thermionic electron gun delivering a thousand momentum-chirped microbunches per macropulse and an alpha-magnet producing microbunches of a sub-mm length. Total radiated energy of a sub-millijoule per a microsecond radio frequency macropulse is demonstrated with flux more than ten micro-Joules per centimeter squared. With 1 THz filter the energy measured is about 1 microjoule and flux of a few micro-Joules per centimeter squared.
The proposed Electron-Ion Collider (EIC) will operate high-luminosity high-energy electron+proton and electron+nucleus collisions at the collision energies from 20 GeV to 141 GeV to solve several fundamental questions in the high energy and nuclear physics fields. Its instantaneous luminosity can reach 10 33-34 cm -2 s -1 and the bunching crossing rate is around 10 ns. The EIC project has received CD1 approval from the US DOE in 2021 and moves toward the machine design and preparation for construction. To realize various particle measurements with high precision at the future EIC, a low material-budget and high-granularity silicon vertex and tracking detector with fine spatial and momentum resolutions and nearly 4π solid angle coverage is desired. The Monolithic Active Pixel Sensor (MAPS) and AC Coupled Low Gain Avalanche Diode (AC-LGAD) technologies stand out of several advanced technology options for the EIC silicon vertex and tracking detector subsystems. The MAPS technology has advanced features of low material budget, low power consumption, good radiation resistance and fine spatial resolution. The AC-LGAD technology can achieve fast timing resolution. Latest studies and progress of the EIC silicon vertex and tracking detector conceptual design, performance validations in simulation and ongoing MAPS and AC-LGAD R&D will be shown. Furthermore, schedule and plan of the EIC project detector development will be discussed as well.
Structural stability of MoS 2 nanosheets were in-situ investigated from selected area electron diffraction. The nano-sheets were stable at low-energy electron irradiation (80 keV) while degraded under high-energy electron irradiation (120 keV).
Magnetotactic bacteria are of great interdisciplinary interest, since a vast field of applications from magnetic recording media to medical nanorobots is conceivable. A key feature for a further understanding is the detailed knowledge about the magnetosome chain within the bacteria. We report on two preparation procedures suitable for UHV experiments in reflective geometry. Further, we present the results of scanning electron microscopy, as well as the first photoemission electron microscopy experiments, both accessing the magnetosomes within intact magnetotactic bacteria and compare these to scanning electron microscopy data from the literature. From the images, we can clearly identify individual magnetosomes within their chains.
Intermetallic compounds represent an extensive pool of candidates for energy related applications stemming from magnetic, electric, optic, caloric, and catalytic properties. The discovery of novel intermetallic compounds can enhance understanding of the chemical principles that govern structural stability and chemical bonding as well as finding new applications. Valence electron-poor polar intermetallics with valence electron concentrations (VECs) between 2.0 and 3.0 e – /atom show a plethora of unprecedented and fascinating structural motifs and bonding features. Furthermore, establishing simple structure-bonding-property relationships is especially challenging for this compound class because commonly accepted valence electron counting rules are inappropriate.
Batteries based on Mg metal anode can promise much higher specific volumetric capacity and energy density compared to Li-ion systems and are, at the same time, safer and more cost-effective. While previous experimental reports have claimed reversible Mg intercalation into beyond Chevrel phase cathodes, they provide limited evidence of true Mg intercalation other than electrochemical data. Transmission electron microscopy techniques provide unique capabilities to directly image Mg intercalation and quantify the redox reaction within the cathode material. Here, we present a systematic study of Mg insertion into orthorhombic V 2 O 5 , combining aberration-corrected scanning transmission electron microscopy (STEM) imaging, electron energy-loss spectroscopy (EELS), and energy-dispersive X-ray spectroscopy (EDX) analysis. We compare the results from an electrochemically cycled V 2 O 5 cathode in a prospective full cell with Mg metal anode with a chemically synthesized MgV 2 O 5 sample. Results suggest that the electrochemically cycled orthorhombic V 2 O 5 cathode shows a local formation of the theoretically predicted ϵ-Mg 0.5 V 2 O 5 phase; however, the intercalation levels of Mg are lower than predicted. Lastly, this phase is different from the chemically synthesized sample, which is found to represent the δ-MgV 2 O 5 phase.
With the arising of global climate change and resource shortage, in recent years, increased attention has been paid to environmentally friendly materials. Trees are sustainable and renewable materials, which give us shelter and oxygen and remove carbon dioxide from the atmosphere. Trees are a primary resource that human society depends upon every day, for example, homes, heating, furniture, and aircraft. Wood from trees gives us paper, cardboard, and medical supplies, thus impacting our homes, school, work, and play. All of the above-mentioned applications have been well developed over the past thousands of years. However, trees and wood have much more to offer us as advanced materials, impacting emerging high-tech fields, such as bioengineering, flexible electronics, and clean energy. Wood naturally has a hierarchical structure, composed of well-oriented microfibers and tracheids for water, ion, and oxygen transportation during metabolism. At higher magnification, the walls of fiber cells have an interesting morphology--a distinctly mesoporous structure. Moreover, the walls of fiber cells are composed of thousands of fibers (or macrofibrils) oriented in a similar angle. Nanofibrils and nanocrystals can be further liberated from macrofibrils by mechanical, chemical, and enzymatic methods. The obtained nanocellulose has unique optical, mechanical, and barrier properties and is an excellent candidate for chemical modification and reconfiguration. Wood is naturally a composite material, comprised of cellulose, hemicellulose, and lignin. Wood is sustainable, earth abundant, strong, biodegradable, biocompatible, and chemically accessible for modification; more importantly, multiscale natural fibers from wood have unique optical properties applicable to different kinds of optoelectronics and photonic devices. Today, the materials derived from wood are ready to be explored for applications in new technology areas, such as electronics, biomedical devices, and energy. The goal of this study is to review the fundamental structures and chemistries of wood and wood-derived materials, which are essential for a wide range of existing and new enabling technologies. The scope of the review covers multiscale materials and assemblies of cellulose, hemicellulose, and lignin as well as other biomaterials derived from wood, in regard to their major emerging applications. Structure-properties-application relationships will be investigated in detail. Understanding the fundamental properties of these structures is crucial for designing and manufacturing products for emerging applications. Today, a more holistic understanding of the interplay between the structure, chemistry, and performance of wood and wood-derived materials is advancing historical applications of these materials. This new level of understanding also enables a myriad of new and exciting applications, which motivate this review. There are excellent reviews already on the classical topic of woody materials, and some recent reviews also cover new understanding of these materials as well as potential applications. This review will focus on the uniqueness of woody materials for three critical applications: green electronics, biological devices, and energy storage and bioenergy.
The synthesis, electronic structure, and characterization via single crystal X-ray diffraction, nuclear magnetic resonance (NMR) spectroscopy, and magnetic susceptibility of (Me4N)2PuCl6 are reported. NMR measurements were performed to both search for the direct 239Pu resonance and to obtain local magnetic and electronic information at the Cl site through 35Cl and 37Cl spectra. No signature of 239Pu NMR was observed. The temperature dependence of the Cl spectra was simulated by diagonalizing the Zeeman and quadrupolar Hamiltonians for 35Cl, 37Cl and 14N isotopes. Electronic structure calculations predict a magnetic ?5 triplet ground state of Pu(IV) in the crystalline electric field of the undistorted PuCl6 octahedron. A tetragonal distortion would result in a very small splitting (20 cm-1) of the triplet ground state into a nonmagnetic singlet and a doublet state. The Cl shifts have an inflection point at T = 15 K, differing from the bulk susceptibility, indicating a nonmagnetic crystal field ground state. The Cl spin-lattice relaxation time is constant down to T = 15 K, below which it rapidly increases, also supporting the nonmagnetic crystal field ground state.
Here, the kinetics of oxidation of organic and inorganic reductants by aqueous iron(IV) ions, Fe IV (H 2 O) 5 O 2+ (hereafter Fe IV aq O 2+ ), are reported. The substrates examined include several water-soluble ferrocenes, hexachloroiridate(III), polypyridyl complexes M(NN) 3 2+ (M = Os, Fe and Ru; NN = phenanthroline, bipyridine and derivatives), HABTS–/ABTS 2– , phenothiazines, Co II (dmgBF 2 ) 2 , macrocyclic nickel(II) complexes, and aqueous cerium(III). Most of the reductants were oxidized cleanly to the corresponding one-electron oxidation products, with the exception of phenothiazines which produced the corresponding oxides in a single-step reaction, and polypyridyl complexes of Fe(II) and Ru(II) that generated ligand-modified products. Fe IV aq O 2+ oxidizes even Ce(III) (E 0 in 1 M HClO 4 = 1.7 V) with a rate constant greater than 10 4 M –1 s –1 . In 0.10 M aqueous HClO 4 at 25 °C, the reactions of Os(phen) 3 2+ (k = 2.5 × 10 5 M –1 s –1 ), IrCl 6 3– (1.6 × 10 6 ), ABTS 2– (4.7 × 10 7 ), and Fe(cp)(C 5 H 4 CH 2 OH) (6.4 × 10 7 ) appear to take place by outer sphere electron transfer (OSET). The rate constants for the oxidation of Os(phen) 3 2+ and of ferrocenes remained unchanged in the acidity range 0.05 < [H+] < 0.10 M, ruling out prior protonation of Fe IV aq O 2+ and further supporting the OSET assignment. A fit to Marcus cross-relation yielded a composite parameter (log k 22 + E 0 Fe /0.059) = 17.2 ± 0.8, where k 22 and E 0 Fe are the self-exchange rate constant and reduction potential, respectively, for the Fe IV aq O 2+ /Fe III aq O + couple. Comparison with literature work suggests k 22 < 10 –5 M –1 s –1 and thus E 0 (Fe IV aq O 2+ /Fe III aq O + ) > 1.3 V. For proton-coupled electron transfer, the reduction potential is estimated at E 0 (Fe IV aq O 2+ , H + /Fe III aq OH 2+ ) ≥ 1.95 V.
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In this work, proton-coupled electron transfer (PCET) was studied for the ground and excited electronic states of a [Ru(terpy)(bpm)(OH 2 )(PF 6 ) 2 ] complex, Ru-bpm. Cyclic voltammetry measurements show that the Ru(II)-aqua moiety undergoes PCET to form a Ru(IV)-oxo moiety in the anodic region, while the bpm ligand undergoes PCET to form bpmH 2 in the cathodic region. The photophysical behavior of Ru-bpm was studied using steady-state and femtosecond transient UV–vis absorption spectroscopy, coupled with density functional theory (DFT) calculations. The lowest-lying excited state of Ru-bpm is described as a (Ru → bpm) metal-to-ligand charge-transfer (MLCT) state, while the metal-centered (MC) excited state was found computationally to be close in energy to the lowest-energy bright MLCT state (MC state was 0.16 eV above the MLCT state). The excited-state kinetics of Ru-bpm were found via transient absorption spectroscopy to be short-lived and were fit well to a biexponential function with lifetimes $τ_1$ = 4 ps and $τ_2$ = 65 ps in aqueous solution. Kinetic isotope effects of 1.75 ($τ_1$) and 1.61 ($τ_2$) were observed for both decay components, indicating that the solvent plays an important role in the excited-state dynamics of Ru-bpm. Based on the pH-dependent studies and the results from prior studies of similar Ru-complexes, we hypothesize that the 3 MLCT state forms an excited-state hydrogen-bond adduct with the solvent molecules and that this process occurs with a 4 ps lifetime. The formation of such a hydrogen-bond complex is consistent with the electronic density accumulation at the peripheral N atoms of the bpm moiety in the 3 MLCT state. The hydrogen-bonded state 3 MLCT decays to the ground state with a 65 ps lifetime. Such a short lifetime is likely associated with the efficient vibrational energy transfer from the 3 MLCT state to the solvent.
We investigate the basis-set-size dependence for quantities related to interacting electrons in the canonical ensemble. Calculations are performed using exact diagonalization (finite temperature full configuration interaction method) on two-electron model systems–the uniform electron gas (UEG) and the helium atom. Our data reproduce previous observations of a competition for how the internal energy converges between the ground-state correlation energy and the high-temperature kinetic energy. We explore how this can be related to component parts of the internal energy including kinetic, exchange, and correlation energies and show there is surprising nuance in how this can be broken down into mostly monotonically converging quantities. We also show that separation of the free energy into a free energy with/without correlation allows for monotonic convergence with basis set size due to the variational principle. We find that the free energy convergence matches the previously observed convergence properties of the internal energy. We discuss the free energy divergence that happens when converging a finite basis analytical hydrogen atom to the complete basis set limit and compare this to the energies of a helium atom in a large periodic box. Reducing the box size, we saw convergence trends for the helium atom that were similar to the UEG.
The electronic properties of dye-sensitized semiconductor surfaces consisting of perylene chromophores chemisorbed on zinc oxide via different spacer-anchor groups have been studied at the density-functional-theory level. The energy distributions of the donor states and the rates of photoinduced electron transfer from dye to surface are predicted. We evaluate in particular the impact of saturated versus unsaturated aliphatic spacer groups inserted between the perylene chromophore and the semiconductor as well as the influence of surface defects on the electron-injection rates.
The exponential computational cost of describing strongly correlated electrons can be mitigated by adopting a reduced-density-matrix (RDM)-based description of the electronic structure. While variational two-electron RDM (v2RDM) methods can enable large-scale calculations on such systems, the quality of the solution is limited by the fact that only a subset of known necessary N-representability constraints can be applied to the 2RDM in practical calculations. Here, we demonstrate that violations of partial three-particle (T1 and T2) N-representability conditions, which can be evaluated with knowledge of only the 2RDM, can serve as physics-based features in a machine-learning (ML) protocol for improving energies from v2RDM calculations that consider only two-particle (PQG) conditions. Proof-of-principle calculations demonstrate that the model yields substantially improved energies, relative to reference values from configuration-interaction-based calculations.
X-ray free electron lasers (XFELs) provide ultrashort intense X-ray pulses suitable to probe electron dynamics but can also induce a multitude of nonlinear excitation processes. These affect spectroscopic measurements and interpretation, particularly for upcoming brighter XFELs. Here we identify and discuss the limits to observing classical spectroscopy, where only one photon is absorbed per atom for a Mn 2+ in a light element (O, C, H) environment. X-ray emission spectroscopy (XES) with different incident photon energies, pulse intensities, and pulse durations is presented. A rate equation model based on sequential ionization and relaxation events is used to calculate populations of multiply ionized states during a single pulse and to explain the observed X-ray induced spectral lines shifts. Furthermore this model provides easy estimation of spectral shifts, which is essential for experimental designs at XFELs and illustrates that shorter X-ray pulses will not overcome sequential ionization but can reduce electron cascade effects.
Oxide–water interfaces are ubiquitous, with many applications in industry and the environment, yet there is a great deal of controversy over their properties and microscopic structure. This controversy stems, in part, from the unique H-bond networks formed at different surface terminations and mineral compositions. Density functional theory simulations of these interfaces require an accurate description of both the oxide mineral and water in diverse H-bond environments. Thus, herein we simulate the Al 2 O 3 (001)–H 2 O interface using the PBE, PBE-TS, RPBE, SCAN, and HSE06-TS functionals to determine how calculated interfacial properties depend on the choice of functional. We find that the structure of the first few layers of water at the surface is determined by electron correlation in a way that cannot be approximated using semiemipirical van der Waals corrections. Of the functionals investigated, we find that SCAN yields the most accurate interfacial structure, dynamics, and sum frequency generation spectrum. Furthermore, SCAN leads to a reduction in the order of the 2D H-bond network of water at the alumina surface predicted by GGA functionals, leading to a significant decrease in the anisotropy of the diffusion coefficient at the surface. We emphasize the importance of using a functional which accurately describes electron correlation for more complex oxides, such as transition-metal oxides, where electron correlation may play an even greater role in determining the structure and dynamics of the oxide–water interface.
Rare earth nickelates including LaNiO3 are promising catalysts for water electrolysis to produce oxygen gas. Recent studies report that Fe substitution for Ni can significantly enhance the oxygen evolution reaction (OER) activity of LaNiO3. However, the role of Fe in increasing activity remains ambiguous, with potential origins both structural and electronic in nature. Here, by utilizing a series of epitaxial LaNi1-xFexO3 thin films synthesized by oxygen-assisted molecular beam epitaxy, we report that Fe substitution tunes the oxidation state of Ni in LaNi1-xFexO3 and a volcano-like OER trend is observed with x = 0.375 being the most active. Spectroscopy and ab initio modeling reveal that the high-valent Fe3+? B-site cationic species strongly increases the transition metal (TM) 3d bandwidth via Ni-O-Fe bridges and enhances the TM 3d-O 2p hybridization, boosting the OER activity. Furthermore, pH-dependent electrochemical measurements suggest that the OER on LaNi1-xFexO3 involves a lattice oxygen-mediated mechanism.