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Understanding hydrogen-metal interactions is important in various fields of surface science, including the aqueous corrosion of metals. The interaction between atomic H and a Mg surface is a key process for the formation of sub-surface Mg hydride, which may play an important role in Mg aqueous corrosion. In the present work, we performed first-principles Density Functional Theory (DFT) calculations to study the mechanisms for hydrogen adsorption and crystalline Mg hydride formation under aqueous conditions. The Electron Localisation Function (ELF) is found to be a promising indicator for predicting stable H adsorption in the Mg surface. It is found that H adsorption and hydride layer formation is dominated by high ELF adsorption sites. Our calculations suggest that the on-surface adsorption of atomic H, OH radicals and atomic O could enhance the electron localisation at specific sites in the sub-surface region, thus forming effective H traps locally. This is predicted to result in the formation of a thermodynamically stable sub-surface hydride layer, which is a potential precursor of the crucial hydride corrosion product of magnesium.

The electronic and spintronic properties of the monovacancies in freestanding and isotopically compressed graphene are investigated using hybrid exchange density functional perturbation theory. When the effects of electronic self-interaction are taken into account, an integer magnetic moment of 2 μ

In many engineering scenarios, surface-active organic species are added to acidic solutions to inhibit the corrosion of metallic components. Given suitable selection, such corrosion inhibitors are highly effective, preventing significant degradation even in highly aggressive environments. Nevertheless, there are still considerable gaps in fundamental knowledge of corrosion inhibitor functionality, severely restricting rational development. Here, we demonstrate the capability of X-ray photoelectron spectroscopy (XPS), supported by ab initio modelling, for revealing key details of inhibited substrates. Attention is focussed on the corrosion inhibition of carbon steel through the addition of an exemplar imidazoline-based corrosion inhibitor (OMID) to aqueous solutions of both HCl and H2SO4. Most notably, it is demonstrated that interfacial chemistry varies with the identity of the acid. High resolution Fe 2p, O 1s, N 1s, and Cl 2p XPS spectra, acquired from well-inhibited carbon steel in 1 M HCl, show that there are two different singly protonated OMID species bound directly to the metallic carbon steel substrate. In sharp contrast, in 0.01 M H2SO4, OMID adsorbs onto an ultra-thin surface film, composed primarily of a ferric sulfate (Fe-2(SO4)(3))-like phase. Such insight is essential to efforts to develop a mechanistic description of corrosion inhibitor functionality, as well as knowledge-based identification of next generation corrosion inhibitors.

Surface adsorption is one of the fundamental processes in numerous fields, including catalysis, environment, energy and medicine. The development of an adsorption model which provides an effective prediction of binding energy in minutes has been a long term goal in surface and interface science. The solution has been elusive as identifying the intrinsic determinants of the adsorption energy for various compositions, structures and environments is non-trivial. We introduce a new and flexible model for predicting adsorption energies to metal substrates. The model is based on easily computed, intrinsic properties of the substrate and adsorbate. It is parameterised using machine learning based on first-principles calculations of probe molecules (e.g., H$_2$O, CO$_2$, O$_2$, N$_2$) adsorbed to a range of pure metal substrates. The model predicts the computed dissociative adsorption energy to metal surfaces with a correlation coefficient of 0.93 and a mean absolute error of 0.77 eV for the large database of molecular adsorption energies provided by \textit{Catalysis-Hub.org} which have a range of 15 eV. As the model is based on pre-computed quantities it provides near-instantaneous estimates of adsorption energies and it is sufficiently accurate to eliminate around 90\% of candidates in screening study of new adsorbates. The model, therefore, significantly enhances current efforts to identify new molecular coatings in many applied research fields., Comment: 11 pages, 7 figures

Perovskites have been widely studied for electrocatalysis due to the exceptional activity they exhibit for surface-mediated redox reactions. To date, descriptors based on density functional theory calculations or experimental measurements have assumed a bulk-like configuration for the surfaces of these oxides. Herein, we probed an initial exposed surface and the screened subsurface of LaMnO3 particles, demonstrating that their augmented activity toward the oxygen reduction reaction (ORR) can be related to a spontaneous surface reconstruction. Our approach involves high energy resolution electron energy loss spectroscopy for the fine structure probing of oxygen and manganese ionization edges under electron beam conditions that leave the structure unaffected. Atomic multiplet and density functional theory calculations were used to compute the theoretical energy loss spectra for comparison to the experimental data, allowing to quantitatively demonstrate that the particle surface layers are La-deficient. This deficiency is linked to equivalent tetrahedral Mn2+ sites at the reconstructed surface, leading to the coexistence of +3 and +2 oxidation states of Mn at the surface layers. This electronic and structural configuration of the as-synthesized particles is indirectly linked to strong adsorption pathways that promote the ORR on LaMnO3, and thus, it could prove to be a valuable design feature in the engineering of catalytic surfaces.

The beam spin asymmetry of the exclusive pseudoscalar channel e → p → e ′ p ′ η was measured for the first time in the deep-inelastic regime ( W > 2 GeV / c 2 and Q 2 > 1 GeV 2 / c 2 ) using a longitudinally polarized 5.78 GeV electron beam at Jefferson Lab with the CEBAF Large Acceptance Spectrometer. The data were accumulated in 144 four-dimensional bins of Q 2 , x B , − t and ϕ over a wide kinematic range, where ϕ is the azimuthal angle between the lepton and hadron scattering planes, The measured azimuthal dependence with large amplitudes of the sin ⁡ ϕ moments is a clear indication of a substantial contribution to the polarized cross-section from transversely polarized virtual photons. In the framework of generalized parton distributions (GPDs) this contribution is expressed via longitudinal-transverse interference between chiral-even and chiral-odd GPDs. The experimental results are compared to the existing theoretical models demonstrating the sensitivity to the product of chiral-odd and chiral-even GPDs and provide new constraints to the existing GPD parameterizations.

Recent interest in functionalized graphene has been motivated by the prospect of creating a two-dimensional semiconductor with a tunable band gap. Various approaches to band gap engineering have been made over the last decade, one of which is chemical functionalization. In this work, a predictive physical model of the self-assembly of halogenated carbene layers on graphene is suggested. Self-assembly of the adsorbed layer is found to be governed by a combination of the curvature of the graphene sheet, local distortions, as introduced by molecular adsorption, and short-range intermolecular repulsion. The thermodynamics of bidental covalent molecular adsorption and the resultant electronic structure are computed using density functional theory. It is predicted that a direct band gap is opened that is tunable by varying coverages and is dependent on the ripple amplitude. This provides a mechanism for the controlled engineering of graphene’s electronic structure and thus its use in semiconductor technologies.

Heterojunction photocatalysts can significantly enhance the efficiency of photocatalytic water splitting. It is well known that the key to such improvements lies at the interfacial region where charge separation occurs. Understanding the origins of this interfacial enhancement can enable the design of better performing water splitting devices. Therefore, in this work, a novel theoretical–experimental approach is developed for the study of photocatalytic heterojunctions using the model system – WO3/BiVO4, where it has been shown that the quantum efficiency of water splitting can approach unity at certain wavelengths. Our photoelectrochemical measurements of this heterojunction show a significantly enhanced performance over its separate components when illuminated through the BiVO4 side but not the WO3 side. This is indicative of more efficient electron transfer (i.e. from BiVO4 to WO3) than hole transfer (i.e. from WO3 to BiVO4) across the junction. Our classical band bending model of this junction predicts noticeable interfacial barriers, but could not explain the reduced performance under back illumination. Our atomistic model was used to investigate the effect of interfacial reconstructions and chemical interactions on the electronic structure of the system. The model reveals a non-staggered valence band, in contrast to the staggered conduction band, due to strong hybridization of valence band orbitals in both materials across the interface. This non-staggered valence band does not provide an energetic driving force for charge separation for hole transfer (i.e. from WO3 to BiVO4 under back illumination). Hence, a significant improvement in performance is only observed under front illumination. This combined approach, using both experiment and theory, results in a more complete understanding of a heterojunction photocatalyst system and provides unique insight into the interfacial effects that arise when two semiconductor materials are brought together, going beyond traditional band bending models.

Photoproduction cross sections are reported for the reaction $\gamma p\to p\eta$ using energy-tagged photons and the CLAS spectrometer at Jefferson Laboratory. The $\eta$ mesons are detected in their dominant charged decay mode, $\eta\to \pi^+\pi^-\pi^0$, and results on differential cross sections are presented for incident photon energies between 1.2 and 4.7 GeV. These new $\eta$ photoproduction data are consistent with earlier CLAS results but extend the energy range beyond the nucleon resonance region into the Regge regime. The normalized angular distributions are compared with the experimental results from several other experiments, and with predictions of $\eta$ MAID\,2018 and the latest solution of the Bonn-Gatchina coupled-channel analysis. Differential cross sections $d\sigma/dt$ are presented for incident photon energies $E_\gamma > 2.9$ GeV ($W > 2.5$ GeV), and compared with predictions which are based on Regge trajectories exchange in the $t$-channel (Regge models). The data confirm the expected dominance of $\rho$, $\omega$ vector-meson exchange in an analysis by the Joint Physics Analysis Center.

A combination of electrochemical measurement and interface analysis have been applied to characterise the interaction of OMID, an exemplar imidazoline-based corrosion inhibitor, with carbon steel in 1 M hydrochloric acid. Corrosion inhibition efficiency data indicate that excellent performance is achieved well below the critical micelle concentration. High resolution X-ray photoelectron spectra demonstrate that, as the corrosion rate decreases, the interface evolves towards one comprising OMID bound to film-free carbon steel. This latter result provides key input for those researchers attempting to predict corrosion inhibitor functionality through atomic scale interfacial modelling, and so identify next generation chemistries.

We have measured beam-spin asymmetries to extract the \ud sin\ud ϕ\ud moment \ud A\ud sin\ud ϕ\ud L\ud U\ud from the hard exclusive \ud →\ud e\ud p\ud →\ud e\ud ′\ud n\ud π\ud +\ud reaction above the resonance region, for the first time with nearly full coverage from forward to backward angles in the center of mass. The \ud A\ud sin\ud ϕ\ud L\ud U\ud moment has been measured up to \ud 6.6\ud \ud \ud GeV\ud 2\ud in \ud −\ud t\ud , covering the kinematic regimes of generalized parton distributions (GPD) and baryon-to-meson transition distribution amplitudes (TDA) at the same time. The experimental results in very forward kinematics demonstrate the sensitivity to chiral-odd and chiral-even GPDs. In very backward kinematics where the TDA framework is applicable, we found \ud A\ud sin\ud ϕ\ud L\ud U\ud to be negative, while a sign change was observed near 90° in the center of mass. The unique results presented in this Letter will provide critical constraints to establish reaction mechanisms that can help to further develop the GPD and TDA frameworks.

We present the first measurement of the exclusive reaction $\gamma p \rightarrow a_2(1320)^0 \, p$ in the photon energy range $3.5$-$5.5$ GeV and four-momentum transfer squared $0.2

Robust fitting of core level photoemission spectra is often central to reliable interpretation of X‐ray photoelectron spectroscopy (XPS) data. One key element is employment of the correct line shape function for each spectral component. In this study, we consider this topic, focusing on XPS data from atomic adsorbates, namely, O and S, on Fe(110). The potential of employing density functional theory (DFT) for generating adsorbate projected electronic density of states (PDOS) to support line shape selection is explored. O 1s core level XPS spectra, acquired from various ordered overlayers of chemisorbed O, all display an equivalent asymmetric line shape. Previous work suggests that this asymmetry is a result of finite O PDOS in the vicinity of the Fermi level, allowing O 1s photoexcitation to induce a weighted continuum of final states through electron‐hole pair excitation. This origin is corroborated by O DFT‐PDOS generated for an optimised five‐layer Fe(110)(2 × 2)‐O slab. Adsorbate DFT‐PDOS were also computed for Fe(110) urn:x-wiley:01422421:media:sia6770:sia6770-math-0001 ‐S. As, similar to adsorbed O, there is a significant continuous distribution of states about the Fermi level, it is proposed that the S 2p XPS core levels should also have asymmetric profiles. S 2p XPS data acquired from Fe(110) urn:x-wiley:01422421:media:sia6770:sia6770-math-0002 ‐S, and their subsequent fitting, verify this prediction, suggesting that DFT‐PDOS could aid line shape selection.

High field magnetization measurements in pulsed fields up to 65 T have been performed on ${\mathrm{FePS}}_{3}$, which is nominally a good example of a two-dimensional Ising-like antiferromagnet on a honeycomb lattice. Measurements with the field parallel to the moment direction confirm the presence of two first-order transitions above 35 T, to $M/{M}_{\mathrm{sat}}=1/2$ and $M/{M}_{\mathrm{sat}}=1$, respectively, at 4 K. The measurements are in contradiction with published estimates for the magnetic exchange parameters, but the contradiction can be resolved by allowing for anisotropic exchange parameters in the Hamiltonian. The magnetization with the field perpendicular to the moment direction is anisotropic, with no transitions observed for fields along the a axis while a cascade of first-order transitions is observed for fields above 50 T along the b axis, the latter case also showing a strong degradation of the sample after repeated pulses. The results indicate a strong magnetolattice coupling in ${\mathrm{FePS}}_{3}$. Temperature-dependent measurements hint at a possible tricritical point.

International audience; The CEBAF Large Acceptance Spectrometer for operation at 12 GeV beam energy (CLAS12) in Hall B at Jefferson Laboratory is used to study electro-induced nuclear and hadronic reactions. This spectrometer provides efficient detection of charged and neutral particles over a large fraction of the full solid angle. CLAS12 has been part of the energy-doubling project of Jefferson Lab’s Continuous Electron Beam Accelerator Facility, funded by the United States Department of Energy. An international collaboration of 48 institutions contributed to the design and construction of detector hardware, developed the software packages for the simulation of complex event patterns, and commissioned the detector systems. CLAS12 is based on a dual-magnet system with a superconducting torus magnet that provides a largely azimuthal field distribution that covers the forward polar angle range up to 35 ∘ , and a solenoid magnet and detector covering the polar angles from 35° to 125° with full azimuthal coverage. Trajectory reconstruction in the forward direction using drift chambers and in the central direction using a vertex tracker results in momentum resolutions of < 1% and < 3%, respectively. Cherenkov counters, time-of-flight scintillators, and electromagnetic calorimeters provide good particle identification. Fast triggering and high data-acquisition rates allow operation at a luminosity of 1035 cm −2 s −1 . These capabilities are being used in a broad program to study the structure and interactions of nucleons, nuclei, and mesons, using polarized and unpolarized electron beams and targets for beam energies up to 11 GeV. This paper gives a general description of the design, construction, and performance of CLAS12.

International audience; We describe offline event reconstruction for the CEBAF Large Acceptance Spectrometer at 12 GeV (CLAS12), including an overview of the offline reconstruction framework and software tools, a description of the algorithms developed for the individual detector subsystems, and the overall approach for charged and neutral particle identification. We also present the scheme for data processing and the code management procedures.

Our understanding of material properties in the broadest sense is based on our ability to observe and disentangle underlying mechanisms. This has been aided enormously by the discovery and exploitation of synchrotron radiation. The next generation of light sources will be based on free electron lasers with potentially much greater light intensity and time resolution. This requires the development of new photocathode materials with high quantum efficiency (QE) and low emittance that are chemically and mechanically robust. One prospect is the use of yttrium (Y) and/or magnesium (Mg) thin films, but here, a fundamental understanding of the photoemission process from realistic materials is lacking. Observations of photoemissive performance would appear to contradict simple models. It is well known that materials with a lower work function are expected to facilitate photoemission, but the measured QE of Mg is higher than that of Y despite its nominal work function (3.7 eV) being significantly higher than that of Y (3.1 eV). In this work, these apparently anomalous observations are explained and rationalized by combining a simple three-step model of photoemission with large scale density functional theory calculations to predict the QE for realistic models of both materials in a special chemical environment. This approach allows us to identify the material parameters that govern the efficiency of the photoemission process. A detailed comparison with the experimental data suggests that, in this case, hydride formation on the Y surface, invisible to most experimental probes, nevertheless has a surprisingly large influence and reduces the photoemission significantly.

We present precision measurements of the target and beam-target spin asymmetries from neutral pion electroproduction in deep-inelastic scattering (DIS) using the CEBAF Large Acceptance Spectrometer (CLAS) at Jefferson Lab. We scattered 6-GeV, longitudinally polarized electrons off longitudinally polarized protons in a cryogenic $^{14}$NH$_3$ target, and extracted double and single target spin asymmetries for $ep\rightarrow e^\prime\pi^0X$ in multidimensional bins in four-momentum transfer ($1.0, Comment: 18 preprint pages, 3 figures

Refractory transition metal nitrides and oxynitrides are of interest for plasmonic applications due to their increased thermal stability, tunability and comparatively low loss. Presented here is an experimental investigation of reactively sputtered niobium oxynitride thin films, demonstrating screened plasma wavelengths tunable over a ~90 nm spectral range. The optical response is correlated with resistivity and Hall measurements. Additionally, an explanation is provided for the double epsilon-near-zero (2ENZ) behavior observed and it is compared with other material systems. Experimental analysis of film composition and structure are combined with computational modelling, based on density functional theory, to explain the dispersion behavior observed and indicate that 2ENZ behavior arises due to the incorporation of oxygen within the films during deposition.

High-momentum configurations of nucleon pairs at short-distance are probed using measurements of the $^{12}$C$(e,e'p)$ and $^{12}$C$(e,e'pN)$ reactions (where $N$ is either $n$ or $p$), at high-$Q^2$ and $x_B>1.1$. The data span a missing-momentum range of 300--1000 MeV/c and are predominantly sensitive to the transition region of the strong nuclear interaction from a Tensor to Scalar interaction. The data are well reproduced by theoretical calculations using the Generalized Contact Formalism with both chiral and phenomenological nucleon-nucleon ($NN$) interaction models. This agreement suggests that the measured high missing-momentum protons up to $1000$ MeV/c predominantly belong to short-ranged correlated (SRC) pairs. The measured $^{12}$C$(e,e'pN)$ / $^{12}$C$(e,e'p)$ and $^{12}$C$(e,e'pp)$ / $^{12}$C$(e,e'pn)$ cross-section ratios are consistent with a decrease in the fraction of proton-neutron SRC pairs and increase in the fraction of proton-proton SRC pairs with increasing missing momentum. This confirms the transition from an isospin-dependent tensor $NN$ interaction at $\sim 400$ MeV/c to an isospin-independent scalar interaction at high-momentum around $\sim 800$ MeV/c as predicted by theoretical calculation., Accepted for publication in Physics Letters B. 7 pages, 3 figures, and online supplementary materials

Photon beam asymmetry Σ measurements for ω photoproduction in the reaction γ → p → ω p are reported for photon energies from 1.152 to 1.876 GeV. Data were taken using a linearly-polarized tagged photon beam, a cryogenic hydrogen target, and the CLAS spectrometer in Hall B at Jefferson Lab. The measurements obtained markedly increase the size of the database for this observable, extend coverage to higher energies, and resolve discrepancies in previously published data. Comparisons of these new results with predictions from a chiral-quark-based model and from a dynamical coupled-channels model indicate the importance of interferences between t-channel meson exchange and s- and u-channel contributions, underscoring sensitivity to the nucleon resonances included in those descriptions. Comparisons with the Bonn–Gatchina partial-wave analysis indicate the Σ data reported here help to fix the magnitudes of the interference terms between the leading amplitudes in that calculation (Pomeron exchange and the resonant portion of the J P = 3 / 2 + partial wave), as well as the resonant portions of the smaller partial waves with J P = 1 / 2 − , 3 / 2 − , and 5 / 2 + .

The thermal and magnetic properties of uranium dioxide, a prime nuclear fuel and thoroughly studied actinide material, remain a long standing puzzle, a result of strong coupling between magnetism and lattice vibrations. The magnetic state of this cubic material is characterized by a 3-k non-collinear antiferromagnetic structure and multidomain Jahn-Teller distortions, likely related to its anisotropic thermal properties. Here we show that single crystals of uranium dioxide subjected to strong magnetic fields along threefold axes in the magnetic state exhibit the abrupt appearance of positive linear magnetostriction, leading to a trigonal distortion. Upon reversal of the field the linear term also reverses sign, a hallmark of piezomagnetism. A switching phenomenon occurs at ±18 T, which persists during subsequent field reversals, demonstrating a robust magneto-elastic memory that makes uranium dioxide the hardest piezomagnet known. A model including a strong magnetic anisotropy, elastic, Zeeman, Heisenberg exchange, and magnetoelastic contributions to the total energy is proposed., The nuclear fuel uranium dioxide is of intrinsic interest due to its industrial applications but it also exhibits intriguing electronic and magnetic properties. Here, the authors demonstrate how its complex magnetic structure and interactions give rise to a strong piezomagnetic effect.

Broken fourfold rotational (C4) symmetry is observed in the experimental properties of several classes of unconventional superconductors. It has been proposed that this symmetry breaking is important for superconducting pairing in these materials, but in the high-Tc cuprates this broken symmetry has never been observed on the Fermi surface. Here we report a pronounced anisotropy in the angle dependence of the interlayer magnetoresistance of the underdoped high transition temperature (high-Tc) superconductor YBa2Cu3O6.58, directly revealing broken C4 symmetry on the Fermi surface. Moreover, we demonstrate that this Fermi surface has C2 symmetry of the type produced by a uniaxial or anisotropic density-wave phase. This establishes the central role of C4 symmetry breaking in the Fermi surface reconstruction of YBa2Cu3O6+δ , and suggests a striking degree of universality among unconventional superconductors. Observations of broken rotational symmetry in YBa2Cu3O6.58 suggest that it could be a universal feature in unconventional superconductors. The origin of superconductivity in materials that do not conform to conventional Bardeen–Cooper–Schrieffer theory remains an important puzzle for condensed matter physicists; one that could hold the key to designing materials that have no resistance near room temperature. An international team of researchers led by Brad Ramshaw used angle-dependent magnetoresistance measurements to directly reveal a broken rotational symmetry on the Fermi surface of underdoped crystals of the copper oxide-based unconventional superconductor YBa2Cu3O6.58. As this feature has been found in several other classes of unconventional superconductors, the authors suggest that this may be a universal feature, which could play an important role in the unconventional formation of superconducting pairs.

Manganese porphyrins are of interest due to the optical, electronic and magnetic properties of the central metal ion, coupled to the low bandgap of the polyaromatic ring. These attractive characteristics are harnessed in solutions or in ultra-thin films, such as, for example, self-assembled monolayers. However, for devices, thicker films deposited using a controlled and reproducible method are required. Here we present the morphological, structural, chemical and optical properties of manganese(III) tetraphenylporphyrin chloride (MnTPPCl) thin films deposited using organic molecular beam deposition, typically employed to process analogue molecules for applications such as organic photovoltaics. We find, using a combination of UV-vis and X-ray photoelectron spectroscopies, that the sublimation process leads to the scission of the Mn–Cl bond. The resultant film is a Mn(II)TPP:Mn(III)TPPCl blend where approximately half the molecules have been reduced. Following growth, exposure to air oxidizes the Mn(II)TPP molecule. Through quantitative analysis of the time-dependent optical properties, the oxygen diffusion coefficient (D) [Formula: see text] is obtained, corresponding to a slow bulk oxidation following fast oxidation of a 8-nm-thick surface layer. The bulk diffusion D is lower than for analogous polycrystalline films, suggestion that grain boundaries, rather than molecular packing, are the rate-limiting steps in oxidation of molecular films. Our results highlight that the stability of the axial ligands should be considered when depositing metal porphyrins from the vapor phase, and offer a solvent-free route to obtain reproducible and smooth thin films of complex materials for engineering film functionalities.

Despite intensive study over many years, the chemistry and physicsof the atomic level mechanisms that govern corrosion are not fully understood. In particular, the occurrence and severity of highly localized metal degradation cannot currently be predicted and often cannot be rationalized in failure analysis. We report a first-principles model of the nature of protective iron carbonate films coupled with a detailed chemical and physical characterization of such a film in a carefully controlled environment. The fundamental building blocks of the protective film, siderite (FeCO3) crystallites, are found to be very sensitive to the growth environment. In iron-rich conditions, cylindrical crystallites form that are highly likely to be more susceptible to chemical attack and dissolution than the rhombohedral crystallites formed in iron-poor conditions. This suggests that local degradation of metal surfaces is influenced by structures that form during early growth and provides new avenues for the prevention, detection, and mitigation of carbon steel corrosion.

Developing the next generation of free-electron lasers (FELs) depends on lowering the work function and increasing the quantum efficiency of the photocathode material. However, rules for designing appropriate materials are difficult to discern from observations of structure-composition relationships. This study uses high-quality electronic-structure calculations and a simple physical model to develop design rules for metallic alloys. Interestingly, Cu-Ba alloys terminating in a plane of Ba atoms bear a significant surface dipole, low work function, and high quantum efficiency. These alloys could yield better photocathodes than conventional Cu, and thus better FEL performance.

First measurements of double-polarization observables in ω photoproduction off the proton are presented using transverse target polarization and data from the CEBAF Large Acceptance Spectrometer (CLAS) FROST experiment at Jefferson Lab. The beam-target asymmetry F has been measured using circularly polarized, tagged photons in the energy range 1200-2700 MeV, and the beam-target asymmetries H and P have been measured using linearly polarized, tagged photons in the energy range 1200-2000 MeV. These measurements significantly increase the database on polarization observables. The results are included in two partial-wave analyses and reveal significant contributions from several nucleon (N^{*}) resonances. In particular, contributions from new N^{*} resonances listed in the Review of Particle Properties are observed, which aid in reaching the goal of mapping out the nucleon resonance spectrum.

We report the first experimental measurements of the nine 1-fold differential cross sections for the γp→π+π−p reaction, obtained with the CLAS detector at Jefferson Laboratory. The measurements cover the invariant mass range of the final state hadrons from 1.6 GeV Δ(1620)1/2−, Δ(1700)3/2−, N(1720)3/2+, and Δ(1905)5/2+ resonances, which have dominant decays into the ππN final states rather than the more extensively studied single meson decay channels.

This paper presents, for the first time, measurements of neutron transparency ratios for nuclei relative to C measured using the (e,e'n) reaction, spanning measured neutron momenta of 1.4 to 2.4 GeV/c. The transparency ratios were extracted in two kinematical regions, corresponding to knockout of mean-field nucleons and to the breakup of Short-Range Correlated nucleon pairs. The extracted neutron transparency ratios are consistent with each other for the two measured kinematical regions and agree with the proton transparencies extracted from new and previous (e,e'p) measurements, including those from neutron-rich nuclei such as lead. The data also agree with and confirm the Glauber approximation that is commonly used to interpret experimental data. The nuclear-mass-dependence of the extracted transparencies scales as A^{\alpha} with {\alpha} = -0.289 {\pm} 0.007, which is consistent with nuclear-surface dominance of the reactions., Comment: Accepted for publication in Physics Letters B

In the past two decades, deeply virtual Compton scattering of electrons has been successfully used to advance our knowledge of the partonic structure of the free proton and investigate correlations between the transverse position and the longitudinal momentum of quarks inside the nucleon. Meanwhile, the structure of bound nucleons in nuclei has been studied in inclusive deep-inelastic lepton scattering experiments off nuclear targets, showing a significant difference in longitudinal momentum distribution of quarks inside the bound nucleon, known as the EMC effect. In this work, we report the first beam spin asymmetry (BSA) measurement of exclusive deeply virtual Compton scattering (DVCS) off a proton bound in $^4$He. The data used here were accumulated using a $6$ GeV longitudinally polarized electron beam incident on a pressurized $^4$He gaseous target placed within the CLAS spectrometer in Hall-B at the Thomas Jefferson National Accelerator Facility. The azimuthal angle ($\phi$) dependence of the BSA was studied in a wide range of virtual photon and scattered proton kinematics. The $Q^2$, $x_B$, and t dependencies of the BSA on the bound proton are compared with those on the free proton. In the whole kinematical region of our measurements, the BSA on the bound proton is smaller by 20\% to 40\%, indicating possible medium modification of its partonic structure.

We measured the triple coincidence A(e,e'np) and A(e,e'pp) reactions on carbon, aluminum, iron, and lead targets at Q2 > 1.5 (GeV/c)2, xB > 1.1 and missing momentum > 400 MeV/c. This was the first direct measurement of both proton-proton (pp) and neutron-proton (np) short-range correlated (SRC) pair knockout from heavy asymmetric nuclei. For all measured nuclei, the average proton-proton (pp) to neutron-proton (np) reduced cross-section ratio is about 6%, in agreement with previous indirect measurements. Correcting for Single-Charge Exchange effects decreased the SRC pairs ratio to ~ 3%, which is lower than previous results. Comparisons to theoretical Generalized Contact Formalism (GCF) cross-section calculations show good agreement using both phenomenological and chiral nucleon-nucleon potentials, favoring a lower pp to np pair ratio. The ability of the GCF calculation to describe the experimental data using either phenomenological or chiral potentials suggests possible reduction of scale- and scheme-dependence in cross section ratios. Our results also support the high-resolution description of high-momentum states being predominantly due to nucleons in SRC pairs., Accepted for publication in PRL. 9 pages, 3 figures, 3 tables and supplementary materials

The doubly strange Xi baryons provide an effective way to study a puzzle called the missing-baryons problem where both quark models and lattice guage theory predict more baryon excited states than are seen experimentally. However, few of these excited states have been observed with any certainty. Here, high-mass Xi* states have been searched for in photoproduction with the detector of the CLAS collaboration, and upper limits for the total cross sections have been established from threshold to W = 3.3 GeV. In addition, the total cross sections of the ground-state Xi(-)(1320) and first excited state Xi(-)(1530) are presented, extending significantly the centre-of-mass energy range of previous data.

Obtaining a bright and low emittance electron beam directly from the photocathode is mandatory in order to design high performance free electron lasers (FELs). To achieve this goal a clear understanding of how the emission process is influenced by structure, morphology and composition of the photocathode surface is needed. This is difficult from an experimental point of view because often the atomic scale details of the surface whose emission has been measured are unknown. A predictive theoretical approach capable of determining the effects of surface structure on emission is therefore or great interest. A model to extend the well known three step model (as proposed by Berglund and Spicer) to surface calculations is discussed in this paper. It is based on a layer-by-layer decomposition of the surface electronic structure that can be calculated through reliable and efficient DFT calculations. The advantage of this approach with respect to other existing photoemission calculations is being able to correlate directly the photoemission to the electronic, atomic and chemical structure of the surface. The proposed approach retains, therefore, the simple chemical intuition in the study of surface modifications and their effect on the photoemission. The approach is validated in calculations of the emission from clean copper and silver surfaces. The ability of the model to simulate the change in photoemission in response to adsorbates is tested by simulating monolayers of oxygen, hydrogen and lithium on the copper (1 1 1) surface.

The observation of a reconstructed Fermi surface via quantum oscillations in hole-doped cuprates opened a path towards identifying broken symmetry states in the pseudogap regime. However, such an identification has remained inconclusive due to the multi-frequency quantum oscillation spectra and complications accounting for bilayer effects in most studies. We overcome these impediments with high-resolution measurements on the structurally simpler cuprate HgBa2CuO4+δ (Hg1201), which features one CuO2 plane per primitive unit cell. We find only a single oscillatory component with no signatures of magnetic breakdown tunnelling to additional orbits. Therefore, the Fermi surface comprises a single quasi-two-dimensional pocket. Quantitative modelling of these results indicates that a biaxial charge density wave within each CuO2 plane is responsible for the reconstruction and rules out criss-crossed charge stripes between layers as a viable alternative in Hg1201. Lastly, we determine that the characteristic gap between reconstructed pockets is a significant fraction of the pseudogap energy., The identification of broken symmetry states in underdoped cuprate superconductors via quantum oscillation measurements remains inconclusive. Here, Chan et al. report the reconstructed Fermi surface of HgBa2CuO4+δ comprises only a single pocket indicating a biaxial charge-density-wave order within each CuO2 plane.

Scanned-energy mode photoelectron diffraction (PhD) and ab initio density functional theory calculations have been employed to investigate the adsorption geometry of benzoate ([C6H5COO]−) on rutile-TiO2(110)(1 × 1). PhD data indicate that the benzoate moiety binds to the surface through both of its oxygen atoms to two adjacent fivefold surface titanium atoms in an essentially upright geometry. Moreover, its phenyl (C6H5−) and carboxylate ([−COO]−) groups are determined to be coplanar, being aligned along the [001] azimuth. This experimental result is consistent with the benzoate geometry emerging from DFT calculations conducted for laterally rather well-separated adsorbates. At shorter interadsorbate distances, the theoretical modeling predicts a more tilted and twisted adsorption geometry, where the phenyl and carboxylate groups are no longer coplanar; i.e., interadsorbate interactions influence the configuration of adsorbed benzoate.

We report the first measurements of the E beam-target helicity asymmetry for the γn→K0Λ and K0Σ0 channels in the energy range 1.70≤W≤2.34 GeV. The CLAS system at Jefferson Lab uses a circularly polarized photon beam and a target consisting of longitudinally polarized solid molecular hydrogen deuteride with low background contamination for the measurements. The multivariate analysis method boosted decision trees is used to isolate the reactions of interest. Comparisons with predictions from the KaonMAID, SAID, and Bonn-Gatchina models are presented. These results will help separate the isospin I=0 and I=1 photocoupling transition amplitudes in pseudoscalar meson photoproduction.

Electrochemical measurements and substrate analysis have been employed to study the corrosion of iron in sweet solution (pH = 6.8, T = 80 °C) over a period of 288 h. Correlated with decreasing corrosion rate, diffraction, microscopy, and spectroscopy data reveal the evolution of adhered sweet corrosion scale. Initially, it is comprised of two phases, siderite and chukanovite, with the latter affording little substrate protection. Subsequently, as the scale becomes highly protective, siderite is the sole component. Notably, siderite crystals are concluded to display a somewhat unexpected habit, which may be a trigger for local breakdown of protective sweet scales.

Short-range correlated (SRC) nucleon pairs are a vital part of the nucleus, accounting for almost all nucleons with momentum greater than the Fermi momentum (k_{F}). A fundamental characteristic of SRC pairs is having large relative momenta as compared to k_{F}, and smaller center of mass (c.m.) which indicates a small separation distance between the nucleons in the pair. Determining the c.m. momentum distribution of SRC pairs is essential for understanding their formation process. We report here on the extraction of the c.m. motion of proton-proton (pp) SRC pairs in carbon and, for the first time in heavier and ansymetric nuclei: aluminum, iron, and lead, from measurements of the A(e,e^{'}pp) reaction. We find that the pair c.m. motion for these nuclei can be described by a three-dimensional Gaussian with a narrow width ranging from 140 to 170 MeV/c, approximately consistent with the sum of two mean-field nucleon momenta. Comparison with calculations appears to show that the SRC pairs are formed from mean-field nucleons in specific quantum states.

New results on the single-differential and fully integrated cross sections for the process γvp→p′π+π- are presented. The experimental data were collected with the CLAS detector at Jefferson Laboratory. Measurements were carried out in the kinematic region of the reaction invariant mass W from 1.3 to 1.825 GeV and the photon virtuality Q2 from 0.4 to 1.0 GeV2. The cross sections were obtained in narrow Q2 bins (0.05 GeV2) with the smallest statistical uncertainties achieved in double-pion electroproduction experiments to date. The results were found to be in agreement with previously available data where they overlap. A preliminary interpretation of the extracted cross sections, which was based on a phenomenological meson-baryon reaction model, revealed substantial relative contributions from nucleon resonances. The data offer promising prospects to improve knowledge on the Q2 evolution of the electrocouplings of most resonances with masses up to ∼1.8 GeV.

An understanding of the interaction of water with the anatase(101) surface is crucial for developing strategies to improve the efficiency of the photocatalytic reaction involved in solar water splitting. Despite a number of previous investigations, it is still not clear if water preferentially adsorbs in its molecular or dissociated form on anatase(101). With the aim of shedding some light on this controversial issue, we report the results of periodic screened-exchange density functional theory calculations of the dissociative, molecular, and mixed adsorption modes on the anatase(101) surface at various coverages. Our calculations support the suggestion that surface-adsorbed OH groups are present, which has been made on the basis of recently measured X-ray photoelectron spectroscopy, temperature-programmed desorption, and scanning tunneling microscopy data. It is also shown that the relative stability of water adsorption on anatase(101), at different configurations, can be understood in terms of a simple model based on the number and nature of the hydrogen bonds formed as well as the adsorbate-induced atomic displacements in the surface layers. These general conclusions are found to be insensitive to the specific choice of approximation for electronic exchange and correlation within the density functional theory. The simple model of water–anatase interactions presented here may be of wider validity in determining the geometry of water–oxide interfaces.

Exclusive photoproduction cross sections have been measured for the process γ p → p π 0 [ e + e − ( γ ) ] with the Dalitz decay final state using tagged photon energies in the range of E γ = 1.275 – 5.425 GeV. The complete angular distribution of the final state π 0 , for the entire photon energy range up to large values of t and u , has been measured for the first time. The data obtained show that the cross section d σ / d t , at mid to large angles, decreases with energy as s − 6.89 ± 0.26 . This is in agreement with the perturbative QCD quark counting rule prediction of s − 7 . Paradoxically, the size of angular distribution of measured cross sections is greatly underestimated by the QCD-based generalized parton distribution mechanism at highest available invariant energy s = 11 GeV 2 . At the same time, the Regge-exchange-based models for π 0 photoproduction are more consistent with experimental data.

The cross section for coherent ω-meson photoproduction off the deuteron has been measured for the first time as a function of the momentum transfer t=(Pγ−Pω)2 and photon energy Eγ using the CLAS detector at the Thomas Jefferson National Accelerator Facility. The cross sections are measured in the energy range 1.4

The observation of unusual metastable behavior in ${\mathrm{Ca}}_{3}{\mathrm{Co}}_{2}{\mathrm{O}}_{6}$ remains an ongoing puzzle. When the magnetic field is increased at certain very slow rates, evenly spaced steps occur in the magnetization and other physical quantities as a function of magnetic field every 1.2 T. The ground state without steps is approached by slow relaxation processes over hours to days. It is a striking example of extremely slow dynamics arising from geometrical frustration in an otherwise clean and long-range ordered system, and its precise description remains controversial. Here we shed light on the mystery by reporting similar behavior in isostructural ${\mathrm{Ca}}_{3}{\mathrm{Co}}_{2\ensuremath{-}x}{\mathrm{Mn}}_{x}{\mathrm{O}}_{6}$, albeit at magnetic field sweep rates that are six orders of magnitude faster than that in ${\mathrm{Ca}}_{3}{\mathrm{Co}}_{2}{\mathrm{O}}_{6}$. We observe these steps not only in the magnetization, but also in the magnetostriction, electric polarization, and magnetocaloric effect. We present a study of metastable behavior in both compounds across seven orders of magnitude of magnetic field sweep rates using unique magnets at the National High Magnetic Field Laboratory. The metastable steps occur for intermediate ranges of magnetic field sweep rates, vanishing or evolving for the fastest and slowest sweep rates. Our data support that these metastable steps are an intrinsic feature of the three-dimensionally frustrated geometry of Ising spins in this structural family and thus narrow the number of applicable models.

The atomic nucleus is made of protons and neutrons (nucleons), that are themselves composed of quarks and gluons. Understanding how the quark-gluon structure of a nucleon bound in an atomic nucleus is modified by the surrounding nucleons is an outstanding challenge. Although evidence for such modification, known as the EMC effect, was first observed over 35 years ago, there is still no generally accepted explanation of its cause. Recent observations suggest that the EMC effect is related to close-proximity Short Range Correlated (SRC) nucleon pairs in nuclei. Here we report the first simultaneous, high-precision, measurements of the EMC effect and SRC abundances. We show that the EMC data can be explained by a universal modification of the structure of nucleons in neutron-proton (np) SRC pairs and present the first data-driven extraction of this universal modification function. This implies that, in heavier nuclei with many more neutrons than protons, each proton is more likely than each neutron to belong to an SRC pair and hence to have its quark structure distorted., Comment: Published in Nature. Total: 21 pages, 9 figures, 10 tables. Main text: 7 pages, 4 figures. Methods section: 1 page. Extended Data: 1 figure, 3 table. Supplementary Materials: 11 pages, 4 figures, 7 tables

Increasing the quantum efficiency (QE) of metal photocathodes is in the design and development of photocathodes for free-electron laser applications. The growth of metal oxide thin films on certain metal surfaces has previously been shown to reduce the work function (WF). Using a photoemission model B. Camino [Comput. Mater. Sci. 122, 331 (2016)CMMSEM0927-025610.1016/j.commatsci.2016.05.025] based on the three-step model combined with density functional theory calculations we predict that the growth of a finite number of MgO(100) or BaO(100) layers on the Ag(100) surface increases significantly the QE compared with the clean Ag(100) surface for a photon energy of 4.7 eV. Different mechanisms for affecting the QE are identified for the different metal oxide thin films. The addition of MgO(100) increases the QE due to the reduction of the WF and the direct excitation of electrons from the Ag surface to the MgO conduction band. For BaO(100) thin films, an additional mechanism is in operation as the oxide film also photoemits at this energy. We also note that a significant increase in the QE for photons with an energy of a few eV above the WF is achieved due to an increase in the inelastic mean-free path of the electrons.

Graphene oxide (GO) is a versatile 2D material whose properties can be tuned by changing the type and concentration of oxygen-containing functional groups attached to its surface. However, a detailed knowledge of the dependence of the chemo/physical features of this material on its chemical composition is largely unknown. We combine classical molecular dynamics and density functional theory simulations to predict the structural and electronic properties of GO at low degree of oxidation and suggest a revision of the Lerf-Klinowski model. We find that layer deformation is larger for samples containing high concentrations of epoxy groups and that correspondingly the band gap increases. Targeted chemical modification of the GO surface appears to be an effective route to tailor the electronic properties of the monolayer for given applications. Our simulations also show that the chemical shift of the C-1s XPS peak allows one to unambiguously characterize GO composition, resolving the peak attribution uncertainty often encountered in experiments.

We show that novel low temperature properties of bulk SmB6, including the sudden growth of the de Haas-van Alphen amplitude (and heat capacity) originating from the bulk at millikelvin temperatures and a previously unreported linear-in-temperature bulk electrical conductivity at liquid helium temperatures, signal the presence of a highly asymmetric nodal semimetal. We show how the highly asymmetric nodal semimetal can be the result of a topological transformation, of the type recently considered by Shen and Fu, occurring in a Kondo lattice with dispersionless f-electron levels and Sm vacancies or other lattice defects. If supported by further data experimental, the existence of a nodal semimetal would cast considerable doubt over a neutral Fermi surface being required to explain the origin of the dHvA effect SmB6., 4 pages including 4 figures