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At least 577 records · Page 32

From Hydrodynamics to Jet Quenching, Coalescence, and Hadron Cascade: A Coupled Approach to Solving the $R_{AA}Ⓧv_{2}$ Puzzle

Hydrodynamics and jet quenching are responsible for the elliptic flow $v_{2}$ and suppression of large transverse momentum ($p_{T}$) hadrons, respectively, two of the most important phenomena leading to the discovery of a strongly coupled quark-gluon plasma in high-energy heavy-ion collisions. A consistent description of the hadron suppression factor $R_{AA}$ and $v_{2}$, especially at intermediate $p_{T}$, however, remains a challenge. We solve this long-standing $R_{AA}Ⓧv_{2}$ puzzle by including quark coalescence for hadronization and final state hadron cascade in the coupled linear Boltzmann transport-hydro model that combines concurrent jet transport and hydrodynamic evolution of the bulk medium. We illustrate that quark coalescence and hadron cascade, two keys to solving the puzzle, also lead to a splitting of $v_{2}$ for pions, kaons, and protons in the intermediate $p_{T}$ region. We demonstrate for the first time that experimental data on $R_{AA}, v_{2}$, and their hadron flavor dependence from low to intermediate and high $p_{T}$ in high-energy heavy-ion collisions can be understood within this coupled framework.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Mechanistic study of direct coupling of CO 2 and C 2 H 4 over atomically dispersed metal at graphene edges

Direct coupling of CO 2 and ethylene (hereinafter DCCE) to acrylic acid is valuable for valorizing CO 2 to manufacture acrylate-derived products. However, previous studies in DCCE have been limited on molecular catalysts with challenges in improving catalytic performance. In this work, we employed density functional theory calculations and ab initio molecular dynamics simulations to investigate the heterogeneous catalysis of DCCE over atomically dispersed metal centers at nitrogen-doped zigzag edge of graphene. Based on competitive adsorption and structural stability, Mo, Cr, V, Ru, and Ni active sites are chosen to explore the reaction kinetics. Here, we find that the activation barriers are determined by the charge redistribution at transition states, which explains the trend of activity for the C-C coupling and the hydrogen transfer, two key steps in DCCE. Furthermore, we show that the intramolecular hydrogen transfer (rate-limiting step) is hindered due to the lack of local coordinate at the active sites. We thus propose to use co-adsorbed water as a “proton-exchanger” following a water-assisted route, and show that the activation barriers are reduced over all metal centers. Particularly, water promotes the hydrogen transfer over metals with strong CO 2 -ethylene co-activation and facile C-C coupling kinetics, which could be considered promising for DCCE. In both mechanisms, the stability of metallactone intermediate can be used to predict the catalytic activity. It is anticipated that the insights from this work can provide guidelines for mimicking well-defined multifunctional active sites in molecular catalysts to design heterogeneous catalysts for such C-C coupling, which advances catalytic utilization of CO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High density Schottky barrier IRCCD sensors for SWIR applications at intermediate temperature

Monolithic 32 x 64 and 64 x 1:128 palladium silicide (Pd2Si) interline transfer infrared charge coupled devices (IRCCDs) sensitive in the 1 to 3.5 micron spectral band were developed. This silicon imager exhibits a low response nonuniformity of typically 0.2 to 1.6% rms, and was operated in the temperature range between 40 to 140 K. Spectral response measurements of test Pd2Si p-type Si devices yield quantum efficiencies of 7.9% at 1.25 microns, 5.6% at 1.65 microns 2.2% at 2.22 microns. Improvement in quantum efficiency is expected by optimizing the different structural parameters of the Pd2Si detectors. The spectral response of the Pd2Si detectors fit a modified Fowler emission model. The measured photo-electric barrier height for the Pd2Si detectors is 0.34 eV and the measured quantum efficiency coefficient, C1, is 19%/eV. The dark current level of Pd2Si Schottky barrier focal plane arrays (FPAs) is sufficiently low to enable operation at intermediate temperatures at TV frame rates. Typical dark current level measured at 120 K on the FPA is 2 nA/sq cm. The operating temperature of the Pd2Si FPA is compatible with passive cooler performance. In addition, high density Pd2Si Schottky barrier FPAs are manufactured with high yield and therefore represent an economical approach to short wavelength IR imaging. A Pd2Si Schottky barrier image sensor for push-broom multispectral imaging in the 1.25, 1.65, and 2.22 micron bands is being studied. The sensor will have two line arrays (dual band capability) of 512 detectors each, with 30 micron center-to-center detector spacing. The device will be suitable for chip-to-chip abutment, thus providing the capability to produce large, multiple chip focal planes with contiguous, in-line sensors.

Elabd, H.↗

EVOLUTION OF INTERMEDIATE-MASS X-RAY BINARIES DRIVEN BY THE MAGNETIC BRAKING OF AP/BP STARS. I. ULTRACOMPACT X-RAY BINARIES

It is generally believed that ultracompact X-ray binaries (UCXBs) evolved from binaries consisting of a neutron star accreting from a low-mass white dwarf (WD) or helium star where mass transfer is driven by gravitational radiation. However, the standard WD evolutionary channel cannot produce the relatively long-period (40–60 minutes) UCXBs with a high time-averaged mass-transfer rate. In this work, we explore an alternative evolutionary route toward UCXBs, where the companions evolve from intermediate-mass Ap/Bp stars with an anomalously strong magnetic field (100–10,000 G). Including the magnetic braking caused by the coupling between the magnetic field and an irradiation-driven wind induced by the X-ray flux from the accreting component, we show that intermediate-mass X-ray binaries (IMXBs) can evolve into UCXBs. Using the MESA code, we have calculated evolutionary sequences for a large number of IMXBs. The simulated results indicate that, for a small wind-driving efficiency f = 10{sup −5}, the anomalous magnetic braking can drive IMXBs to an ultra-short period of 11 minutes. Comparing our simulated results with the observed parameters of 15 identified UCXBs, the anomalous magnetic braking evolutionary channel can account for the formation of seven and eight sources with f = 10{sup −3}, and 10{sup −5}, respectively. In particular, a relatively large value of f can fit three of the long-period, persistent sources with a high mass-transfer rate. Though the proportion of Ap/Bp stars in intermediate-mass stars is only 5%, the lifetime of the UCXB phase is ≳2 Gyr, producing a relatively high number of observable systems, making this an alternative evolutionary channel for the formation of UCXBs.

79 ASTRONOMY AND ASTROPHYSICS↗

Near-barrier fusion of {sup 32}S+{sup 90,96}Zr: The effect of multi-neutron transfers in sub-barrier fusion reactions

Fusion excitation functions have been measured for the first time with rather good accuracy for {sup 32}S+{sup 90}Zr and {sup 32}S+{sup 96}Zr near and below the Coulomb barrier. The sub-barrier cross sections for {sup 32}S+{sup 96}Zr are much larger than for {sup 32}S+{sup 90}Zr. A coupled-channels calculation considering the inelastic excitations is capable of describing sub-barrier enhancement only for {sup 32}S+{sup 90}Zr. The unexplained part for {sup 32}S+{sup 96}Zr is found to be correlated with the positive-Q-value intermediate neutron transfers in this system. The comparison with {sup 40}Ca+{sup 96}Zr suggests that couplings to the positive-Q-value neutron transfer channels may play a role in the sub-barrier fusion enhancement. Multi-neutron transfers are taken into account in Zagrebaev's semiclassical model to explain the discrepancies of the sub-barrier fusion cross sections for {sup 32}S+{sup 96}Zr.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DUST DYNAMICS IN PROTOPLANETARY DISK WINDS DRIVEN BY MAGNETOROTATIONAL TURBULENCE: A MECHANISM FOR FLOATING DUST GRAINS WITH CHARACTERISTIC SIZES

We investigate the dynamics of dust grains of various sizes in protoplanetary disk winds driven by magnetorotational turbulence, by simulating the time evolution of the dust grain distribution in the vertical direction. Small dust grains, which are well-coupled to the gas, are dragged upward with the upflowing gas, while large grains remain near the midplane of a disk. Intermediate-size grains float near the sonic point of the disk wind located at several scale heights from the midplane, where the grains are loosely coupled to the background gas. For the minimum mass solar nebula at 1 au, dust grains with size of 25–45 μm float around 4 scale heights from the midplane. Considering the dependence on the distance from the central star, smaller-size grains remain only in an outer region of the disk, while larger-size grains are distributed in a broader region. We also discuss the implications of our result for observations of dusty material around young stellar objects.

79 ASTRONOMY AND ASTROPHYSICS↗

Extending the Kawai-Kerman-McVoy Statistical Theory of Nuclear Reactions to Intermediate Structure via Doorways

Kawai, Kerman, and McVoy have shown that a statistical treatment of many open channels that are coupled by direct reactions leads to modifications of the Hauser- Feshbach expression for energy-averaged cross section (Ann. of Phys. 75 (1973) 156). The energy averaging interval for this cross section is on the order of the width of single particle resonances, 1MeV, revealing only a gross structure in the cross section. When the energy-averaging interval is decreased down to a width of a doorway state 0.1 MeV, a so-called intermediate structure may be observed in cross sections. We extend the Kawai-Kerman-McVoy theory into the intermediate structure by leveraging a theory of doorway states developed by Feshbach, Kerman, and Lemmer (Ann. of Phys. 42 (1967) 230). As a byproduct of the extension, an alternative derivation of the central result of the Kawai-Kerman-McVoy theory is suggested. We quantify the effect of the approximations used in derivation by performing numerical computations for a large set of compound nuclear states.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A study of modal coupling procedures for the space shuttle

Various procedures for analytically coupling two or more substructures to obtain modal data for assembly, using data obtained from mode surveys of the individual components are discussed. Particular attention was paid to the applicability of the techniques investigated to the space shuttle, with the possible replacement of full scale mode surveys of the shuttle assembly by component mode surveys along with analytical coupling. The synthesis procedures formulated in this report can all handle redundant connections, although the presence of redundancies does add complication to one of the techniques. All of the procedures use the test data directly, without going through an intermediate analytical model, and no analytical stiffness data is required to supplement the mode survey data. The coupling precedures were initially verified and evaluated by applying them to analytical check problems.

Goldenberg, S.↗

Data-guided Multi-Map variables for ensemble refinement of molecular movies

Driving molecular dynamics simulations with data-guided collective variables offer a promising strategy to recover thermodynamic information from structure-centric experiments. In this study, the three-dimensional electron density of a protein, as it would be determined by cryo-EM or x-ray crystallography, is used to achieve simultaneously free-energy costs of conformational transitions and refined atomic structures. Unlike previous density-driven molecular dynamics methodologies that determine only the best map-model fits, our work employs the recently developed Multi-Map methodology to monitor concerted movements within equilibrium, non-equilibrium, and enhanced sampling simulations. Construction of all-atom ensembles along the chosen values of the Multi-Map variable enables simultaneous estimation of average properties, as well as real-space refinement of the structures contributing to such averages. Using three proteins of increasing size, we demonstrate that biased simulation along the reaction coordinates derived from electron densities can capture conformational transitions between known intermediates. The simulated pathways appear reversible with minimal hysteresis and require only low-resolution density information to guide the transition. The induced transitions also produce estimates for free energy differences that can be directly compared to experimental observables and population distributions. The refined model quality is superior compared to those found in the Protein Data Bank. We find that the best quantitative agreement with experimental free-energy differences is obtained using medium resolution density information coupled to comparatively large structural transitions. Practical considerations for probing the transitions between multiple intermediate density states are also discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Capaciflector camera

A capacitive type proximity sensor having improved range and sensitivity between a surface and an intruding object in the vicinity of the surface having a voltage source, a number of outer electrical conductors on the surface with each forming one electrode of a number of sensor capacitors, the other electrode for each sensor capacitor being the object is described. The outer conductors are made from thin sheets of conductive material covered with insulation. An intermediate electrical conductor is located between the outer conductors and the surface and is of a size larger than the outer conductors to act as a shield for reducing the parasitic capacitance between the outer conductors and the surface. The intermediate conductor is also made from a thin sheet of conductive material covered with insulation. The outer conductors and the intermediate conductor are attached to the surface with no gap between the insulation on the conductors and no gap between the surface and the insulation on intermediate conductor, the outer conductors and the intermediate conductor conjoining with each other and with the surface, with the surface acting as a ground plane. A current-measuring voltage follower circuit is connected to the voltage source for coupling in phase and amplitude the instantaneous voltage at the voltage source to the outer electrical conductors and the intermediate electrical conductor. This circuit is responsive to the change in capacitance of the sensor capacitors and generates a number of output signals.

Vranish, John M.↗

Capaciflector camera

A capacitive type proximity sensor having improved range and sensitivity between a surface and an intruding object in the vicinity of the surface having a voltage source, a number of outer electrical conductors on the surface with each forming one electrode of a number of sensor capacitors, the other electrode for each sensor capacitor being the object. The outer conductors are made from thin sheets of conductive material covered with insulation. An intermediate electrical conductor is located between the outer conductors and the surface and is of a size larger than the outer conductors to act as a shield for reducing the parasitic capacitance between the outer conductors and the surface. The intermediate conductor is also made from a thin sheet of conductive material covered with insulation. The outer conductors and the intermediate conductor are attached to the surface with no gap between the insulation on the conductors and no gap between the surface and the insulation on intermediate conductor, the outer conductors and the intermediate conductor conjoining with each other and with the surface, with the surface acting as a ground plane. A current-measuring voltage follower circuit is connected to the voltage source for coupling in phase and amplitude the instantaneous voltage at the voltage source to the outer electrical conductors and the intermediate electrical conductor. This circuit is responsive to the change in capacitance of the sensor capacitors and generates a number of output signals.

Vranish, John M.↗

High resolution ENDOR spectroscopy combined with quantum chemical calculations reveals the structure of the nitrogenase Janus intermediate E4(4H)

We have shown that the key state in N2 reduction to two NH3 by the enzyme nitrogenase is the E4(4H), ‘Janus’ intermediate, which has accumulated four [e-/H+] and is poised to undergo reductive elimination of H2 coupled to N2 binding and activation. Initial 1H and 95Mo ENDOR studies of freeze-trapped E4(4H) revealed the catalytic multi-metallic cluster (FeMo-co) binds two Fe-bridging hydrides, [Fe-H-Fe]. However, the analysis failed to provide a satisfactory picture of structure - the relative spatial relationships of the two [Fe-H-Fe]. Our recent density functional theory (DFT) study yielded a lowest-energy form, denoted E4(4H)(a), with two parallel Fe-H-Fe planes bridging pairs of ‘anchor’ Fe on the Fe2,3,6,7 face of FeMo-co. However, the relative energies of structures E4(4H)(b), with one bridging and one terminal hydride, and E4(4H)(c), with one pair of anchor Fe supporting two bridging hydrides, were not beyond the uncertainties of the calculation. Moreover, a structure of V-dependent nitrogenase resulted in a proposed structure analogous to E4(4H)(c), and additional structures have been proposed by DFT studies of others. To resolve the nature of hydride binding to the Janus intermediate, we performed exhaustive, high-resolution CW-stochastic 1H-ENDOR experiments using improved instrumentation, Mims 2H ENDOR, and a pulsed-ENDOR protocol (‘PESTRE’) to obtain absolute hyperfine-interaction signs. These measurements are coupled to DFT structural models through an analytical point-dipole Hamiltonian for the hydride electron-nuclear dipolar coupling to its ‘anchoring’ Fe ions, an approach that overcomes limitations inherent in both experimental interpretation and computational accuracy. The result: the freeze-trapped, lowest-energy Janus intermediate structure is E4(4H)(a).

Hoeke, Veronica↗

Spontaneous Aerosol Ejection: Origin of Inorganic Particles in Biomass Pyrolysis

At high thermal flux and temperatures of approximately 500 °C, lignocellulosic biomass transforms to a reactive liquid intermediate before evaporating to condensable bio-oil for downstream upgrading to renewable fuels and chemicals. However, the existence of a fraction of nonvolatile compounds in condensed bio-oil diminishes the product quality and, in the case of inorganic materials, catalyzes undesirable aging reactions within bio-oil. In this study, ablative pyrolysis of crystalline cellulose was evaluated, with and without doped calcium, for the generation of inorganic-transporting aerosols by reactive boiling ejection from liquid intermediate cellulose. Further, aerosols were characterized by laser diffraction light scattering, inductively coupled plasma spectroscopy, and high-speed photography. Pyrolysis product fractionation revealed that approximately 3 % of the initial feed (both organic and inorganic) was transported to the gas phase as aerosols. Large bubble-to-aerosol size ratios and visualization of significant late-time ejections in the pyrolyzing cellulose suggest the formation of film bubbles in addition to the previously discovered jet formation mechanism.

09 BIOMASS FUELS↗

The changing nature of hydroclimatic risks across South Africa

We present results from large ensembles of projected twenty-first century changes in seasonal precipitation and near-surface air temperature for the nation of South Africa. These ensembles are a result of combining Monte Carlo projections from a human-Earth system model of intermediate complexity with pattern-scaled responses from climate models of the Coupled Model Intercomparison Project Phase 5 (CMIP5). These future ensemble scenarios consider a range of global actions to abate emissions through the twenty-first century. We evaluate distributions of surface-air temperature and precipitation change over three sub-national regions: western, central, and eastern South Africa. In all regions, we find that without any emissions or climate targets in place, there is a greater than 50% likelihood that mid-century temperatures will increase threefold over the current climate’s two-standard deviation range of variability. However, scenarios that consider more aggressive climate targets all but eliminate the risk of these salient temperature increases. A preponderance of risk toward decreased precipitation (3 to 4 times higher than increased) exists for western and central South Africa. Strong climate targets abate evolving regional hydroclimatic risks. Under a target to limit global climate warming to 1.5 °C by 2100, the risk of precipitation changes within South Africa toward the end of this century (2065–2074) is commensurate to the risk during the 2030s without any global climate target. Thus, these regional hydroclimate risks over South Africa could be delayed by 30 years and, in doing so, provide invaluable lead-time for national efforts to prepare, fortify, and/or adapt.

54 ENVIRONMENTAL SCIENCES↗

Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study

In this study, we have investigated the effect of molecular shape and charge asymmetry on the translation dynamics of confined hydrocarbon molecules having different shapes but similar kinetic diameters, inside ZSM-5 pores using molecular dynamics simulations. The mean square displacement of propane, acetonitrile, acetaldehyde, and acetone in ZSM-5 exhibit two different regimes – ballistic and diffusive/sub-diffusive. All the molecules except propane exhibit sub-diffusive motion at time scales greater than 1 ps. The intermediate scattering functions reveal that there is a considerable rotational-translational coupling in the motion of all the molecules, due to the strong geometrical restriction imposed by ZSM-5. Overall the difference in shape and asymmetry in charge imposes severe restriction inside the ZSM-5 channels for all the molecules to different extents. Additionally, the behavior of molecules confined in ZSM-5 in the present study, quantified wherever possible, is compared to their behavior in bulk or in other porous media reported in literature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Metastable Li 1+δ Mn 2 O 4 (0 ≤ δ ≤ 1) Spinel Phases Revealed by in Operando Neutron Diffraction and First-Principles Calculations

Here, we examine the reaction mechanisms driven by the lithiation of Li 1+δ Mn 2 O 4 (0 ≤ δ ≤ 1) spinels via in operando neutron powder diffraction (NPD). New reaction mechanisms are proposed involving solid-solution regions within both cubic and tetragonal spinel phases in addition to a continuous phase transition between them. In operando NPD is an ideal tool to follow the light elements such as lithium and oxygen in cathode materials which are often the key to fully understand their structural evolutions. Here, we report a novel methodology to prepare an extremely thick electrode with ~378 mg·cm –2 loading density suitable for the in operando NPD studies. Enabled by such thick electrode, we find that the metal oxygen M–O (M = Li and Mn) bond lengths in both end members LiMn 2 O 4 and Li 2 Mn 2 O 4 experience pronounced changes larger than dictated by the change in lattice parameters because of the locally formed Jahn–Teller distorted Mn 3+ . First-principles density functional theory calculations confirm these metastable intermediates and further propose atomistic reaction pathways for the phase transition by coupling a global structure search algorithm. In conclusion, these findings redefine the conventional understandings on two-phase reactions of this spinel material.

36 MATERIALS SCIENCE↗

Four-wave mixing in a three-level bichromatic electromagnetically induced transparency system

We investigate the four-wave mixing (FWM) phenomenon in a three-level bichromatic electromagnetically induced transparency system. Theoretical results predict that the FWM will exhibit a multipeak structure under bichromatic coupling fields. The stronger the coupling fields are, the more FWM the peaks should exhibit. Results of an experiment carried out with cold {sup 87}Rb atoms in a magneto-optical trap agree with the theoretical prediction.

74 ATOMIC AND MOLECULAR PHYSICS↗