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At least 1,585 records · Page 88

Extended x-ray emission times of clusters in intense x-ray pulses

Novel experimental spectroscopic and imaging techniques have been developed to exploit x-ray free-electron laser (XFEL) for studying structure and dynamic of non-periodic entities at atomic spatial resolution and femtosecond timescales.Recently, intensity correlation of x-ray fluorescence, based on the principle introduced by Hanbury Brown and Twiss [R. Hanbury Brown and R. Q. Twiss, Nature (London) 177, 27 (1956)], has been proposed for high-resolution imaging of a three-dimensional arrangement of atoms. To explore the applicability of this fluorescence approach, we theoretically investigate fluorescence dynamics of nonperiodic systems subject to x-ray free electron laser (XFEL) pulses over a range of fluences from the linear to nonlinear x-ray absorption regimes as a function of system size, from a single atom to a cluster of 149 171 atoms. Fluorescence dynamics in the nonlinear x-ray regime differs from that in the weak x-ray field in that intense x-ray pulses interrupt the fluorescence dynamics by multiphoton absorption creating a dense electron environment within the sample on a femtosecond timescale. In large systems, the presence of both recombination and photoionization pathways gives rise to an enhanced Kα and Kα h emission yield and an extended emission time beyond the lifetime of the core-excited states. Our analysis suggests that, in an intense x-ray pulse, the Kα h emission line can be a good candidate for fluorescence imaging as it has a higher yield and an emission time that is short relative to the x-ray-induced lattice distortion time.

74 ATOMIC AND MOLECULAR PHYSICS↗

Bogoliubov Fermi surfaces in spin-$\frac{1}{2}$ systems: Model Hamiltonians and experimental consequences

Bogoliubov Fermi surfaces (BFSs) are topologically protected regions of zero energy excitations in a superconductor whose dimension equals that of the underlying normal state Fermi surface. Examples of Hamiltonians exhibiting this “ultranodal” phase are known to preserve charge-conjugation ($\textit{C}$) and parity ($\textit{P}$) but break time-reversal ($\textit{T}$). In this work, we provide examples of model Hamiltonians that do not necessarily preserve this symmetry pattern but have well-defined sign-changing Pfaffians yielding BFSs. While their topological character has not been recognized previously, some of the models we present have been extensively studied in prior literature. Here, we further examine thermodynamic and electronic properties arising from the ultranodal state. In particular, we study the effect of a weak Zeeman field close to the topological transition and propose distinguishing features of BFSs using residual specific heat and tunneling conductance. Our calculation of the superfluid density in a toy multiband model indicates a window of interband pairing strength where BFSs are stable with a positive superfluid density. We also present additional signatures of BFSs in spin-polarized spectral weight and total magnetization measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A Ce-Doped LiI Scintillator Film-Based High Rate, High Spatial Resolution Neutron Anger Camera for Neutron Scattering Facilities

The 2-D position sensitive neutron detectors featuring a significantly improved count rate capacity and a sub-mm spatial resolution are in high demand by neutron scattering facilities, especially the next generation high-flux spallation neutron sources (SNSs). They are anticipated to play a crucial role in fully utilizing the unprecedentedly high neutron brightness offered by these sources. In this work, a high rate and high spatial resolution neutron Anger camera has been successfully developed based on a Ce-doped microcolumnar LiI scintillator film and the PETsys TOFPET2 ASIC readout electronics. The performance evaluation was conducted in a standard laboratory environment as well as the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) with regard to light yield, γ-ray sensitivity, neutron detection efficiency, count rate capability, spatial resolution, and position linearity. The LiI:Ce scintillator was found to have a higher light yield and a lower γ-ray sensitivity than GS20 (i.e., 11729 versus 6000 photons/n and 1.67 × 10 −5 versus on the order of 10 −4 ). The neutron detection efficiency was measured to be 63% at 4.2 Å. This camera demonstrated an exceptional count rate capability, up to at least 481 kHz without rate loss. The spatial resolution was as good as 0.47 mm. Here, the position linearity was also enhanced.

High rate↗

A Plasma Modeling Hierarchy and Verification Approach

This report reviews a hierarchy of formal mathematical models for describing plasma phenomena. Starting with the Boltzmann equation, a sequence of approximations and modeling assumptions can be made that progressively reduce to the equations for magnetohydrodynamics. Understanding the assumptions behind each of these models and their mathematical form is essential to appropriate use of each level of the hierarchy. A sequence of moment models of the Boltzmann equation are presented, then focused into a generalized three-fluid model for neutral species, electrons, and ions. This model is then further reduced to a two-fluid model, for which Braginskii described a useful closure. Further reduction of the two-fluid model yields a Generalized Ohm's Law model, which provides a connection to magnetohydrodynamic approaches. A verification approach based on linear plasma waves is presented alongside the model hierarchy, which is intended as an initial and necessary but not sufficient step for verification of plasma models within this hierarchy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nuclear Data to Reduce Uncertainties in Reactor Antineutrino Measurements

The large quantities of antineutrinos produced through the decay of fission fragments in nuclear reactors provide an opportunity to study the properties of these particles and investigate their use in reactor monitoring. The reactor antineutrino spectra are measured using specialized, large area detectors that detect antineutrinos through inverse beta decay, electron elastic scattering, or coherent elastic neutrino nucleus scattering; although, inverse beta decay is the only demonstrated method so far. Reactor monitoring takes advantage of the differences in the antineutrino yield and spectra resulting from uranium and plutonium fission providing an opportunity to estimate the fissile material composition in the reactor. Recent experiments reveal a deviation between the measured and calculated antineutrino flux and spectra (the reactor anomaly) indicating either the existence of yet undiscovered neutrino physics, uncertainties in the reactor source term calculation, incorrect nuclear data, or a combination of all three. To address the nuclear data that impact the antineutrino spectrum calculations and measurements, an international group of over 180 experts in antineutrino physics, reactor analysis, detector development, and nuclear data came together during the Workshop on Nuclear Data for Reactor Antineutrino Measurements (WoNDRAM) to discuss nuclear data needs and achieve concordance on a set of recommended priorities for nuclear data improvements. Three topical sessions focused on the reactor source term, the antineutrino spectrum, and the detector response, provided a forum to gain consensus amongst the participants on the most important data improvements to address two goals: 1) understand the reactor anomaly and 2) improve the ability to monitor reactors using antineutrinos. This report summarizes the outcomes of the workshop discussions and the recommendations for nuclear data efforts that reduce reactor antineutrino measurement uncertainties.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Electron-stimulated desorption study of hydrogen-exposed aluminum films

H2 adsorption of evaporated clean and H2-exposed aluminum films is investigated by using the electron-stimulated desorption (ESD) method. A strong H(+)ESD signal is observed on a freshly evaporated aluminum surface which is clean according to previously proposed cleanlines criteria. An increased H(+) yield on H2 exposure is also observed. However, the increasing rate of H(+) emission could be directly correlated with small increases in H2O partial pressure during H2 exposure. It is proposed that the oxidation of aluminum by water vapor and subsequent adsorption of H2 or water is the primary process of the enhanced high H(+) yield during H2 exposure.

Park, CH.↗

Rydberg states of helium - A new recoil term

It is shown that the mass-polarization shift in the energy levels of 1sNL Rydberg states of helium contains a term of second order, in the ratio of the electron mass to that of the nucleus, that is independent of L. The derivation of this new recoil term, based on the method of Drachman (1986), is very simple. It yields a correction of significance for the calculation of absolute ionization energies.

Drachman, Richard J.↗

Low noise HgCdTe 128 x 128 SWIR FPA for Hubble space telescope

Large area focal plane arrays of unprecedented performance were developed for use in Near Infrared Camera and Multi-Object Spectrometer (NICMOS), a proposed Hubble Space Telescope refurbishment instrument. These FPAs are 128x128-element, HgCdTe hybrid arrays with a cutoff wavelength of 2.5 microns. The multiplexer consists of a CMOS field effect transistor switch array with a typical mean readout noise of less than 30 electrons. The detectors typically have a mean dark current of less than 10 electrons/s at 77 K, with currents below 2 electrons measured at 60 K (both at 0.5 V reverse bias). The mean quantum efficiency is 40 to 60 percent at 77 K for 1.0 to 2.4 microns. Functional pixel yield is typically greater than 99 percent, and the power consumption is approximately 0.2 mW (during readout only).

Blessinger, Michael↗

Photonics: Technology project summary

Photonics involves the use of light (photons) in conjunction with electronics for applications in communications, computing, control, and sensing. Components used in photonic systems include lasers, optical detectors, optical wave guide devices, fiber optics, and traditional electronic devices. The goal of this program is to develop hybrid optoelectronic devices and systems for sensing, information processing, communications, and control. It is hoped that these new devices will yield at least an order of magnitude improvement in performance over existing technology. The objective of the program is to conduct research and development in the following areas: (1) materials and devices; (2) networking and computing; (3) optical processing/advanced pattern recognition; and (4) sensing.

Depaula, Ramon P.↗

Plasma properties and magnetic field structure of the solar corona, based on coordinated Max 1991 observations from SERTS, the VLA, and magnetographs

The purposes of this investigation are to determine the plasma properties and magnetic field structure of the solar corona using coordinated observations obtained with NASA/GSFC's Solar EUV rocket Telescope and Spectrograph (SERTS), the Very Large Array (VLA), and magnetographs. The observations were obtained under the auspices of NASA's Max '91 program. The methods of achieving the stated purposes of this investigation are: (1) to use SERTS spectra and spectroheliograms to determine coronal plasma properties such as temperature, density, and emission measure; (2) to use the coronal plasma properties to calculate the intensity of the thermal bremsstrahlung microwave emission from the coronal plasma (the minimum microwave intensity expected from the emitting plasma); (3) to establish which emission mechanism(s) contribute to the observed microwave emission by comparing the calculated thermal bremsstrahlung intensity with the observed microwave intensity; (4) to derive the coronal magnetic field for regions in which gyroemission contributes to the microwave emission by determining the appropriate harmonic of the local electron gyrofrequency; (5) to derive the coronal magnetic field for regions in which thermal bremsstrahlung emission alone is responsible for the observed microwave emission by calculating the magnetic field which yields the observed microwave polarization; (6) to derive three-dimensional models of the coronal plasma and magnetic field which are consistent with all of the EUV spectra and spectroheliograms, as well as with the intensity and polarization maps at all of the microwave observing frequencies; and (7) to compare the coronal magnetic field derived from the coordinated multiwaveband observations with extrapolations from photospheric magnetograms.

Brosius, Jeffrey W.↗

Design of a Microwave Assisted Discharge Inductive Plasma Accelerator

The design and construction of a thruster that employs electrodeless plasma preionization and pulsed inductive acceleration is described. Preionization is achieved through an electron cyclotron resonance discharge that produces a weakly-ionized plasma at the face of a conical theta pinch-shaped inductive coil. The presence of the preionized plasma allows for current sheet formation at lower discharge voltages than those employed in other pulsed inductive accelerators that do not employ preionization. The location of the electron cyclotron resonance discharge is controlled through the design of the applied magnetic field in the thruster. Finite element analysis shows that there is an arrangement of permanent magnets that yields a small volume of resonant magnetic field at the coil face. Preionization in the resonant zone leads to current sheet formation at the coil face, which minimizes the initial inductance of the pulse circuit and maximizes the potential electrical efficiency of the accelerator. A magnet assembly was constructed around an inductive coil to provide structural support to the selected arrangement of neodymium magnets. Measured values of the resulting magnetic field compare favorably with the finite element model.

Hallock, Ashley K.↗

Distributed Antenna-Coupled Transition Edge Sensors

We describe progress toward realizing a new architecture for focal plane arrays for the Submillimeter and Far- Infrared (FIR) bands. This architecture is based on a detector design utilizing distributed hot{electron transition edge sensors (TES) coupled to slot antenna elements. Arrays utilizing this type of detector can be considerably easier to manufacture than membrane-isolated TES arrays, because the need for micro-machining is eliminated. We present background and rationale for this new array architecture and details of a new antenna design for an imaging polarimeter, which yields greater bandwidth than past designs. In addition, we describe a cryogenic facility for testing these arrays.

bolometer↗

Nanoporous Iridium Nanosheets for Polymer Electrolyte Membrane Electrolysis

The growth of the hydrogen economy is predicated on advancements in electrochemical energy technologies, with water electrolysis as a key component to the technological portfolio. Much of the focus on anode catalyst development for polymer electrolyte membrane water electrolyzers (PEMWE) is centered on activity as controlled by compositional and morphological impacts on reactant/intermediate/product adsorption. However, the effectiveness of this strategy is found to be limited upon integration of these materials into PEMWE membrane electrode assemblies (MEA). Regardless of catalyst activity, the combination of electrode inhomogeneity, ionomer integration, and high density of oxide-oxide interfaces yields significant performance losses associated with poor catalytic electrode conductivity. Here many of these limitations are addressed through the development of a unique catalyst morphology composed of nanoporous Ir nanosheets (npIr(x)-NS) that exhibit high catalytic activity for the anodic oxygen evolution reaction and superior electrode electronic conductivity in comparison to a commercial IrO2 nanoparticle catalyst. The utility of the npIr(x)-NS is demonstrated through incorporation into PEMWE MEAs where their performance exceeds that of commercial catalyst coated membranes at loadings as low as 0.06 mg(Ir) cm(-2) while exhibiting a negligible loss in performance following 50 000 accelerated stress test cycles.

Polymer Electrolyte Membrane Electrolysis↗

Elucidating Photoinduced Processes of Photosystem I Via Multidimensional Electronic and Vibrational Spectroscopies

This project was motivated by an overarching goal to elucidate the mechanism of energy and electron transfer that governs the efficient charge separation in photosystem I (PSI) complexes. PSI is a natural light harvesting complex that drives oxygenic photosynthesis in plants, algae, and cyanobacteria. It uses ~300 tightly packed chlorophylls (Chls) to absorb photons, transfer the excitation energy to the reaction center (RC), and generate a charge separated state with near unity quantum efficiency (QE). A better understanding of the mechanism of energy transfer and charge separation in PSI is required for understanding the high QE of natural light harvesting complexes, and it could lead to the further development of artificial photosynthetic systems for solar energy conversion and modification of light harvesting complexes to improve crop yields. We applied two-dimensional optical spectroscopies to different cyanobacterial photosystem I complexes, including PSI complexes that contain Chl f molecules, to map energy transfer pathways and gain insight into the efficient light harvesting of PSI. We used two-dimensional electronic spectroscopies (2DES) to map energy transfer in Chl a and Chl f containing PSI complexes. To investigate the Chl f PSI complexes, we modified our spectrometer to probe the lower energy states associated with Chl f molecules. We interpreted the 2DES spectra through global analysis procedures to generate maps of energy transfer. We also constructed a two-dimensional electronic vibrational (2DEV) spectrometer that will be used to investigate charge transfer transitions and dynamics within PSI complexes. Measurements were performed on model systems to establish general data analysis procedures for interpreting 2D spectra and gain insight into protein cofactor interactions.

14 SOLAR ENERGY↗

Heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(s)

The heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) (eq 1) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(S) (eq 2) were investigated over the temperature range 223-296 K in a flow-tube reactor coupled to a quadrupole mass spectrometer. Either a chemical ionization mass spectrometer (CIMS) or an electron-impact ionization mass spectrometer (EIMS) was used to provide suitable detection sensitivity and selectivity. In order to mimic atmospheric conditions, partial pressures of HNO3 and N2O5 in the range 6 x 10(exp -8) - 2 x 10(exp -6) Torr were used. Granule sizes and surface roughness of the solid NaCl substrates were determined by using a scanning electron microscope. For dry NaCl substrates, decay rates of HNO3 were used to obtain gamma(1) = 0.013 +/- 0.004 (1sigma) at 296 K and > 0.008 at 223 K, respectively. The error quoted is the statistical error. After all corrections were made, the overall error, including systematic error, was estimated to be about a factor of 2. HCl was found to be the sole gas-phase product of reaction 1. The mechanism changed from heterogeneous reaction to predominantly physical adsorption when the reactor was cooled from 296 to 223 K. For reaction 2 using dry salts, gamma(2) was found to be less than 1.0 x 10(exp -4) at both 223 and 296 K. The gas-phase reaction product was identified as ClNO2 in previous studies using an infrared spectrometer. An enhancement in reaction probability was observed if water was not completely removed from salt surfaces, probably due to the reaction of N2O5(g) + H2O(s) yields 2HNO3(g). Our results are compared with previous literature values obtained using different experimental techniques and conditions. The implications of the present results for the enhancement of the hydrogen chloride column density in the lower stratosphere after the El Chichon volcanic eruption and for the chemistry of HCl and HNO3 in the marine troposphere are discussed.

Leu, Ming-Taun↗

Modular Wide-bandgap String Inverters for Low-cost Medium-voltage Transformerless PV Systems

The proposed technology combines advances in wide-bandgap power electronics with breakthroughs in distributed and decentralized control to produce ultra-low-cost medium-voltage transformerless PV inverters that are composed of stackable lightweight blocks. Taken together, the proposed circuit designs and accompanying control strategies will yield integrated control+circuit (C2) blocks, each comprising a converter and local controller, that can be assembled in a modular fashion to obtain distributed conversion interfaces for next-generation commercial and utility-scale PV systems. We will utilize SiC devices to obtain C2 blocks that can individually operate at a voltage and power in excess of 1 kV and 100 kW, respectively, such that ensembles of series-connected blocks perform direct dc to three-phase ac conversion at medium voltages (e.g., 12 kV–35 kV) and at multi-MW power levels.

42 ENGINEERING↗

Tetracene Functionalized Si(111) Achieves Enhanced Solar-to-Chemical Energy Conversion via Molecular Acceptor States

The properties of semiconductor|liquid interfaces play a critical role in determining the efficiency of solar-to-hydrogen (STH) conversion. Here, we investigate how molecular functionalization of Si(111) and Si(111)|TiO 2 surfaces impacts photoelectrochemical (PEC) hydrogen production efficiency. We find that functionalization of ∼3% of the atop sites of Si(111) with either 9-anthracene (Anth) or 5-tetracene (Tet), with the remaining sites passivated by methyl groups, provides substrates with high electronic quality and low surface oxide densities, as determined by X-ray photoelectron spectroscopy (XPS) measurements. Surface photovoltage (SPV) spectroscopy shows that surfaces modified with Anth or Tet exhibit an increased photovoltage, with Tet-functionalized surfaces yielding an additional 192 meV relative to methyl-terminated Si(111), indicating improved charge separation for Si-Tet. Further improvement in onset potential was achieved by replacing a nitrogen-containing TiO 2 atomic layer deposition (ALD) precursor (TDMAT) with a precursor lacking nitrogen (TTIP), which eliminates the parasitic defect band in the TiO 2 overlayer (p-Si(111)-Tet|TTIP-TiO 2 |Pt: V OC = +0.283 ± 0.041 V vs RHE). Density functional theory (DFT) analysis demonstrates that compared with Anth-modified Si(111), the Tet-modified surface exhibits more hybridized Si(111)-Tet states closer to the silicon band edges. Mercury contact current–voltage (I–V, dark) measurements quantified the relative interfacial density of states of Si-Tet, Si-Anth and Si-Me surfaces─revealing that the interfacial state density was highest for Si-Tet. This suggests that such hybridized interfaces serve to capture better photoexcited charge, which enables facile electron transfer to molecular acceptors in solution. Altogether, the data indicate that beneficial hybrid molecular LUMO surface states interacting with the Si conduction band edge results in improved hydrogen evolution (HER) performance for p-Si devices.

Group theory↗

Investigating Abiotic and Biotic Mechanisms of Pyrite Reduction

Pyrite (FeS 2 ) has a very low solubility and therefore has historically been considered a sink for iron (Fe) and sulfur (S) and unavailable to biology in the absence of oxygen and oxidative weathering. Anaerobic methanogens were recently shown to reduce FeS 2 and assimilate Fe and S reduction products to meet nutrient demands. However, the mechanism of FeS 2 mineral reduction and the forms of Fe and S assimilated by methanogens remained unclear. Thermodynamic calculations described herein indicate that H 2 at aqueous concentrations as low as 10 –10 M favors the reduction of FeS 2 , with sulfide (HS – ) and pyrrhotite (Fe 1–x S) as products; abiotic laboratory experiments confirmed the reduction of FeS 2 with dissolved H 2 concentrations greater than 1.98 × 10 –4 M H 2 . Growth studies of Methanosarcina barkeri provided with FeS 2 as the sole source of Fe and S resulted in H 2 production but at concentrations too low to drive abiotic FeS 2 reduction, based on abiotic laboratory experimental data. A strain of M. barkeri with deletions in all [NiFe]-hydrogenases maintained the ability to reduce FeS 2 during growth, providing further evidence that extracellular electron transport (EET) to FeS 2 does not involve H 2 or [NiFe]-hydrogenases. Physical contact between cells and FeS 2 was required for mineral reduction but was not required to obtain Fe and S from dissolution products. The addition of a synthetic electron shuttle, anthraquinone-2,6-disulfonate, allowed for biological reduction of FeS 2 when physical contact between cells and FeS 2 was prohibited, indicating that exogenous electron shuttles can mediate FeS 2 reduction. Here, transcriptomics experiments revealed upregulation of several cytoplasmic oxidoreductases during growth of M. barkeri on FeS 2 , which may indicate involvement in provisioning low potential electrons for EET to FeS 2 . Collectively, the data presented herein indicate that reduction of insoluble FeS 2 by M. barkeri occurred via electron transfer from the cell surface to the mineral surface resulting in the generation of soluble HS – and mineral-associated Fe 1–x S. Solubilized Fe(II), but not HS – , from mineral-associated Fe 1–x S reacts with aqueous HS – yielding aqueous iron sulfur clusters (FeS aq ) that likely serve as the Fe and S source for methanogen growth and activity. FeS aq nucleation and subsequent precipitation on the surface of cells may result in accelerated EET to FeS 2 , resulting in positive feedback between cell activity and FeS 2 reduction.

59 BASIC BIOLOGICAL SCIENCES↗