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At least 1,639 records · Page 91

Photoproduction of two charged pions off protons in the resonance region

Photoproduction of charged pions pairs off protons is studied within the invariant masses of the final state hadrons from 1.6 to 2.4 GeV at the Thomas Jefferson National Accelerator Facility with the CLAS detector. The total and differential cross sections and spin-density matrix elements are presented for the isobars pρ 0 (770), Δ(1232) ++ π − , and Δ(1232) 0 π + . The data are included in the Bonn-Gatchina coupled-channel analysis and provide the information necessary to determine the branching fractions of Nρ(770) decays for most known N* and Δ* resonances. For the first time, the Nρ branching ratios are obtained here from an event-based likelihood to γp → π + π − p.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Non-adiabatic molecular dynamics of molecules in the presence of strong light-matter interactions

When the interaction between a molecular system and confined light modes in an optical or plasmonic cavity is strong enough to overcome the dissipative process, hybrid light-matter states (polaritons) become the fundamental excitations in the system. The mixing between the light and matter characters modifies the photophysical and photochemical properties. Notably, it was reported that these polaritons can be employed to control photochemical reactions, charge and energy transfer, and other processes. In addition, according to recent studies, vibrational strong coupling can be employed to resonantly enhance the thermally-activated chemical reactions. In this work, a theoretical model and an efficient numerical method for studying the dynamics of molecules strongly interacting with quantum light are developed based on nonadiabatic excited-state molecular dynamics. The methodology was employed to study the cis-trans photoisomerization of a realistic molecule in a cavity. Numerical simulations demonstrate that the photochemical reactions can be controlled by tuning the properties of the cavity. In the calculated example, the isomerization is suppressed when polaritonic states develop a local minimum on the lower polaritonic state. Moreover, the observed reduction of isomerization is tunable via the photon energy and light-molecule coupling strength. However, the fluctuation in the transition dipole screens the effect of light-matter, which makes it harder to tune the photochemical properties via the coupling strength. These insights gained from this study suggest quantum control of photochemical reactions is possible by specially designed photonic or plasmonic cavities.

36 MATERIALS SCIENCE↗

CO oxidation on gold-supported iron oxides: New insights into strong oxide–metal interactions

Very active FeO x –Au catalysts for CO oxidation are obtained after depositing nanoparticles of FeO, Fe 3 O 4 , and Fe 2 O 3 on a Au(111) substrate. Neither FeO nor Fe 2 O 3 is stable under the reaction conditions. Under an environment of CO/O 2 , they undergo oxidation (FeO) or reduction (Fe 2 O 3 ) to yield nanoparticles of Fe 3 O 4 that are not formed in a bulk phase. Using a combined experimental and theoretical approach, we show a strong oxide–metal interaction (SOMI) between Fe 3 O 4 nanostructures and Au(111), which gives the oxide special properties, allows the formation of an active phase, and provides a unique interface to facilitate a catalytic reaction. This work highlights the important role that the SOMI can play in enhancing the catalytic performance of the oxide component in metal–oxide catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strong Metal–Support Interactions between Copper and Iron Oxide during the High‐Temperature Water‐Gas Shift Reaction

Abstract The commercial high‐temperature water‐gas shift (HT‐WGS) catalyst consists of CuO‐Cr 2 O 3 ‐Fe 2 O 3 , where Cu functions as a chemical promoter to increase the catalytic activity, but its promotion mechanism is poorly understood. In this work, a series of iron‐based model catalysts were investigated with in situ or pseudo in situ characterization, steady‐state WGS reaction, and density function theory (DFT) calculations. For the first time, a strong metal‐support interaction (SMSI) between Cu and FeO x was directly observed. During the WGS reaction, a thin FeO x overlayer migrates onto the metallic Cu particles, creating a hybrid surface structure with Cu‐FeO x interfaces. The synergistic interaction between Cu and FeO x not only stabilizes the Cu clusters, but also provides new catalytic active sites that facilitate CO adsorption, H 2 O dissociation, and WGS reaction. These new fundamental insights can potentially guide the rational design of improved iron‐based HT‐WGS catalysts.

Zhu, Minghui↗

Tip‐Enhanced Imaging and Control of Infrared Strong Light‐Matter Interaction

Optical antenna resonators enable control of light‐matter interactions on the nano‐scale via electron–photon hybrid states in strong coupling. Specifically, mid‐infrared (MIR) nano‐antennas coupled to saturable intersubband transitions in multi‐quantum‐well (MQW) semiconductor heterostructures allow for the coupling strength to be tuned through antenna resonance and field intensity. Here, in this study, tip‐enhanced nano‐scale variation of antenna‐MQW coupling across the antenna is demonstrated, with a spatially‐dependent coupling strength $g_{\textrm{aq}}$ varying from 73 (strong coupling) to 24 cm -1 (weak coupling). This behavior is modeled based on the spatially dependent local constructive and destructive interference between tip and antenna fields. Using a quantum‐mechanical density‐matrix model of the MQW system with its designed values of transition dipole moment, doping density, and population decay time, the picosecond IR pulse coupling to intersubband transitions and the associated tip induced strong‐field saturation effects are described. These results present a new regime of nonlinear IR light‐matter control based on the dynamic manipulation of quantum hybrid states on the nanoscale and in the infrared, with a perspective regarding extension to molecular vibrations.

Wang, Yueying↗

Development of an efficient analysis for high Reynolds number inviscid/viscid interactions in cascades

An efficient steady analysis for predicting strong inviscid/viscid interaction phenomena such as viscous-layer separation, shock/boundary-layer interaction, and trailing-edge/near-wake interaction in turbomachinery blade passages is described. It uses an inviscid/viscid interaction approach, wherein the flow in the outer inviscid region is assumed to be potential, and that in the inner or viscous-layer region is governed by Prandtl's equations. The inviscid solution is determined using an implicit, least-squares, finite-difference approximation. The viscous-layer solution is obtained using an inverse, finite-difference, space-marching method which is applied along the blade surfaces and the wake streamline. A semiinverse global iteration procedure permits the prediction of boundary-layer separation and other strong-interaction phenomena. Results are presented for two cascades where a range of inlet flow conditions was considered for one of them including conditions leading to large-scale flow separation.

Barnett, M.↗

An analysis for high Reynolds number inviscid/viscid interactions in cascades

An efficient steady analysis for predicting strong inviscid/viscid interaction phenomena such as viscous-layer separation, shock/boundary-layer interaction, and trailing-edge/near-wake interaction in turbomachinery blade passages is needed as part of a comprehensive analytical blade design prediction system. Such an analysis is described. It uses an inviscid/viscid interaction approach, in which the flow in the outer inviscid region is assumed to be potential, and that in the inner or viscous-layer region is governed by Prandtl's equations. The inviscid solution is determined using an implicit, least-squares, finite-difference approximation, the viscous-layer solution using an inverse, finite-difference, space-marching method which is applied along the blade surfaces and wake streamlines. The inviscid and viscid solutions are coupled using a semi-inverse global iteration procedure, which permits the prediction of boundary-layer separation and other strong-interaction phenomena. Results are presented for three cascades, with a range of inlet flow conditions considered for one of them, including conditions leading to large-scale flow separations. Comparisons with Navier-Stokes solutions and experimental data are also given.

Barnett, Mark↗

Dependency of CO 2 methanation on the strong metal-support interaction for supported Ni/CeO 2 catalysts

The strong metal-support interaction (SMSI) for supported Ni/CeO 2 catalysts with different CeO 2 nanomorphologies was systematically explored. The degree of encapsulation of Ni particles originating from the SMSI effect was found to follow the trend of Ni/CeO 2 -(1 1 1) > Ni/CeO 2 -(1 0 0) > Ni/CeO 2 -(110 + 100), which parallels the CO 2 hydrogenation activity. Quasi in situ XPS reveals the presence of Ce 3+ sites in accordance with the formation of an amorphous surface CeOx layer encapsulating the Ni nanoparticles. In situ DRIFTS indicates the reaction pathway and rate-determining step are dependent on the degree of the SMSI effect, leading to distinct selectivities towards CH 4 , especially at a high weight hourly space velocity (WHSV). Finally, these findings present a fundamental strategy about tailoring catalytic performance through support facet dependent susceptibility of SMSI phenomena.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Clathrate BaNi 2 P 4 : An Interplay of Heat and Charge Transport Due to Strong Host–Guest Interactions

Heat and charge transport properties of the metallic unconventional clathrate BaNi 2 P 4 , hosting Ba cations in oversized Ni 8 P 16 cages, are investigated. A novel method of single-crystal growth was developed, yielding 2–3 mm sized crystals of BaNi 2 P 4 . We also developed a setup to accurately measure thermal conductivity and electrical resistivity of the synthesized single crystals in a wide temperature range avoiding crystal remounting. BaNi 2 P 4 has a metallic temperature dependence of its electrical resistivity (decreasing with decreasing temperature) and manifests an unconventional T 2 power law for 50 K < T < 300 K; below 50 K, the power-law exponent increases gradually such that below 10 K the power law is T 5 , a predicted but extremely rarely experimentally observed dependence for peculiar electron–phonon interactions. Furthermore, electronic band structure calculations, consistent with measurements of de Haas–van Alphen oscillations, show large band dispersions with significant contributions of Ba orbitals to states near the Fermi level, which is atypical for clathrates. The thermal properties of BaNi 2 P 4 were probed using a combination of variable-temperature single-crystal X-ray diffraction experiments, heat capacity measurements, first-principles phonon dispersion calculations, and inelastic neutron scattering measurements. BaNi 2 P 4 exhibits significant hybridization of the Ba-guest and Ni–P-framework vibrational modes, which may be enhanced via the detected split of the Ba position, which results in strong Ba-framework interactions.

36 MATERIALS SCIENCE↗

Experimental Observations of Laser-Driven Tin Ejecta Microjet Interactions

The study of high-velocity particle-laden flow interactions is of importance for the understanding of a wide range of natural phenomena, ranging from planetary formation to cloud interactions. Experimental observations of particle dynamics are sparse given the difficulty of generating high-velocity flows of many particles. Ejecta microjets are micron-scale jets formed by strong shocks interacting with imprinted surfaces to generate particle plumes traveling at several kilometers per second. As such, the interaction of two ejecta microjets provides a novel experimental methodology to study interacting particle streams. In this Letter, we report the first time sequences of x-ray radiography images of two interacting tin ejecta microjets taken on a platform designed for the OMEGA Extended Performance (OMEGA EP) laser. We observe that the microjets pass through each other unattenuated for the case of 11.7±3.2 GPa shock pressures and jet velocities of 2.2±0.5 km/s but show strong interaction dynamics for 116.0±6.1 GPa shock pressures and jet velocities of 6.5±0.5 km/s. Furthermore, we find that radiation-hydrodynamic simulations of the experiments are able to capture many aspects of the collisional behavior, such as the attenuation of jet velocity in the direction of propagation, but are unable to match the full spread of the strongly interacting cloud.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Strong ferromagnetic exchange interaction under ambient pressure in BaFe 2 S 3

Inelastic neutron scattering measurements have been performed to investigate the spin waves of the quasi-one-dimensional antiferromagnetic ladder compound BaFe 2 S 3 , where a superconducting transition was observed under pressure [H. Takahashi et al., Nat. Mater. 14, 1008 (2015); T. Yamauchi et al., Phys. Rev. Lett. 115, 246402 (2015)]. By fitting the spherically averaged experimental data collected on a powder sample to a Heisenberg Hamiltonian, we find that the one-dimensional antiferromagnetic ladder exhibits a strong nearest-neighbor ferromagnetic exchange interaction (SJ R = - 71 ± 4 meV) along the rung direction, an antiferromagnetic SJ L = 49 ± 3 meV along the leg direction, and a ferromagnetic SJ 2 = - 15 ± 2 meV along the diagonal direction. Finally, our data demonstrate that the antiferromagnetic spin excitations are a common characteristic for the iron-based superconductors, while specific relative values for the exchange interactions do not appear to be unique for the parent states of the superconducting materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Communication: An adaptive configuration interaction approach for strongly correlated electrons with tunable accuracy

We introduce a new procedure for iterative selection of determinant spaces capable of describing highly correlated systems. This adaptive configuration interaction (ACI) determines an optimal basis by an iterative procedure in which the determinant space is expanded and coarse grained until self-consistency. Two importance criteria control the selection process and tune the ACI to a user-defined level of accuracy. The ACI is shown to yield potential energy curves of N{sub 2} with nearly constant errors, and it predicts singlet-triplet splittings of acenes up to decacene that are in good agreement with the density matrix renormalization group.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dynamical observation and detailed description of catalysts under strong metal–support interaction

Understanding the structures of catalysts under realistic conditions with atomic precision is crucial to design better materials for challenging transformations. Under reducing conditions, certain reducible supports migrate onto supported metallic particles and create strong metal–support states that drastically change the reactivity of the systems. The details of this process are still unclear and preclude its thorough exploitation. Here, we report an atomic description of a palladium/titania (Pd/TiO 2 ) system by combining state-of-the-art in situ transmission electron microscopy and density functional theory (DFT) calculations with structurally defined materials, in which we visualize the formation of the overlayers at the atomic scale under atmospheric pressure and high temperature. We show that an amorphous reduced titania layer is formed at low temperatures, and that crystallization of the layer into either mono- or bilayer structures is dictated by the reaction environment and predicted by theory. Moreover, it occurs in combination with a dramatic reshaping of the metallic surface facets.

36 MATERIALS SCIENCE↗

Interaction of a strong blast wave with a free surface

When a point source explosion is initiated at the ocean surface, the shock propagated into the water is reflected at the surface as a centered expansion wave. The solution in the neighborhood of the interaction point is obtained by writing the equations of motion in the appropriate similarity variables and then changing the independent variables to polar coordinates based at the interaction point. From the zero-order solution of the resulting equations the slopes of boundaries at the interaction point are obtained. A first-order perturbation of this solution provides more accurate representation of the flow variables and the curvature of the shock surface near the interaction point.

Falade, A.↗

Correlating furfural reaction pathways with interactions between furfural and monometallic surfaces

Controlling the selectivity of furfural reaction is an important step towards valorizing this important platform chemical in biomass conversion. Previous studies speculate that the selectivity of furfural reaction depends on the interactions of furan ring with metal surfaces. In this work, high resolution electron energy loss spectroscopy (HREELS) and temperature programmed desorption (TPD) are employed to directly study the correlations between furfural reaction pathways and interactions between furfural and different monometallic surfaces. Monometallic surfaces with strong ring interactions favor ring-opening products, while monometallic surfaces with weak ring interactions favor furan production. Oxophilic metal surface like Fe(110) promotes the hydrodeoxygenation pathway to produce 2-methylfuran due to strong interaction with the carbonyl group. Furthermore, these results should provide guidance in the future catalyst design for converting furfural to value-added products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Single-hole physics in GaAs/AlGaAs double quantum dot system with strong spin–orbit interaction

There is rapidly expanding interest in exploiting the spin of valence-band holes rather than conduction-band electrons for spin qubit semiconductor circuits composed of coupled quantum dots. The hole platform offers stronger spin–orbit interaction (SOI), large difference between in-dot-plane and out-of-dot-plane g-factors, i.e. g-factor anisotropy, and a significantly reduced hyperfine coupling to nuclei in the host material. These attributes collectively can deliver fast all-electric coherent spin manipulation, efficient spin-flip inter-dot tunneling channels, a voltage tunable effective g-factor, a g-factor adjustable to nearly zero in an appropriately oriented external magnetic field, and long spin relaxation and coherence times. In this work, we review our recent work on the physics of heavy holes confined in a planar GaAs/AlGaAs double quantum dot system with strong SOI. For a single-hole, we have performed resonant tunneling magneto-spectroscopy to extract spin-flip and spin-conserving tunneling strengths, implemented spin-flip Landau–Zener–Stückelberg–Majorana (LZSM) interferometry, determined the spin relaxation time T 1 as a function of magnetic field using a fast single-shot latched charge technique, electrically tuned the effective g-factor revealed by electric dipole spin resonance, and found signatures of the hyperfine interaction and dynamic nuclear polarization with holes. For two-holes, we have measured the energy spectrum in the presence of strong SOI (and so not limited by Pauli spin blockade), quantified the heavy-hole (HH) g-factor anisotropy on tilting the magnetic field, described a scheme to employ HHs whose g-factor is tunable to nearly zero for an in-plane magnetic field for a coherent photon-to-spin interface, and observed a well-defined LZSM interference pattern at small magnetic fields on pulsing through the singlet-triplet anti-crossing.

74 ATOMIC AND MOLECULAR PHYSICS↗

Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

The optimization of supported metal catalysts predominantly focuses on engineering the metal site, for which physical insights based on extensive theoretical and experimental contributions have enabled the rational design of active sites. Although it is well known that supports can influence the catalytic properties of metals, insights into how metal–support interactions can be exploited to optimize metal active-site properties are lacking. Here in this paper, we utilize in situ spectroscopy and microscopy to identify and characterize a support effect in oxide-supported heterogeneous Rh catalysts. This effect is characterized by strongly bound adsorbates (HCO x ) on reducible oxide supports (TiO 2 and Nb 2 O 5 ) that induce oxygen-vacancy formation in the support and cause HCO x -functionalized encapsulation of Rh nanoparticles by the support. The encapsulation layer is permeable to reactants, stable under the reaction conditions and strongly influences the catalytic properties of Rh, which enables rational and dynamic tuning of CO 2 -reduction selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗