Ambient-Pressure X-ray Photoelectron Spectroscopy to Characterize the Solid/Liquid Interface: Probing the Electrochemical Double Layer

Ambient-pressure X-ray photoelectron spectroscopy (APXPS) has contributed greatly to a wide range of research fields, including environmental science [1 H. Bluhm, Journal of Electron Spectroscopy and Related Phenomena 177, 71–84 (2010).[Crossref], [Web of Science ®] , [Google Scholar]], catalysis [2 D.E. Starr et al., Chemical Society Reviews 42, 5833–5857 (2013).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]], and electrochemistry [3 E.J. Crumlin, H. Bluhm, and Z. Liu, Journal of Electron Spectroscopy and Related Phenomena 190, 84–92 (2013).[Crossref], [Web of Science ®] , [Google Scholar]], to name a few. The use of this technique at synchrotron facilities primarily focused on probing the solid/gas interface; however, it quickly advanced to the probing of liquid/vapor interfaces [4 D.E. Starr et al., Physical Chemistry Chemical Physics 10, 3093–3098 (2008).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar], 5 M.A. Brown et al., Physical Chemistry Chemical Physics 10, 4778–4784 (2008).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]] and solid/liquid interfaces through an X-ray-transparent window [6 J. Kraus et al., Nanoscale 6, 14394–14403 (2014).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]–8 T. Masuda et al., Appl Phys Lett 103 (2013).[Crossref], [Web of Science ®] , [Google Scholar]]. Most recently, combining APXPS with “Tender” X-rays (~2.5 keV to 8 keV) on beamline 9.3.1 at the Advanced Light Source in Lawrence Berkeley National Laboratory (which can generate photoelectrons with much longer inelastic mean free paths) has enabled us to probe the solid/liquid interface without needing a window [9 S. Axnanda et al., Scientific Reports 5 (2015).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]]. This innovation allows us to probe interfacial chemistries of electrochemically controlled solid/liquid interfaces undergoing charge transfer reactions [9 S. Axnanda et al., Scientific Reports 5 (2015).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]]. These advancements have transitioned APXPS from a traditional surface science tool to an essential interface science technique.     

Emergent <Emphasis Type=Italic>SO</Emphasis>(3) Symmetry of the Frictionless Shear Jamming Transition

We study the shear jamming of athermal frictionless soft spheres, and find that in the thermodynamic limit, a shear-jammed state exists with different elastic properties from the isotropically-jammed state. For example, shear-jammed states can have a non-zero residual shear stress in the thermodynamic limit that arises from long-range stress-stress correlations. As a result, the ratio of the shear and bulk moduli, which in isotropically-jammed systems vanishes as the jamming transition is approached from above, instead approaches a constant. Despite these striking differences, we argue that in a deeper sense, the shear jamming and isotropic jamming transitions actually have the same symmetry, and that the differences can be fully understood by rotating the six-dimensional basis of the elastic modulus tensor.     

Coupled nonlinear size-dependent behaviour of microbeams

The nonlinear resonant behaviour of a microbeam, subject to a distributed harmonic excitation force, is investigated numerically taking into account the longitudinal as well as the transverse displacement. Hamilton’s principle is employed to derive the coupled longitudinal-transverse nonlinear partial differential equations of motion based on the modified couple stress theory. The discretized form of the equations of motion is obtained by applying the Galerkin technique. The pseudo-arclength continuation technique is then employed to solve the discretized equations of motion numerically. Different types of bifurcations as well as the stability of solution branches are determined. The numerical results are presented in the form of frequency-response and force-response curves for different sets of parameters. The effect of taking into account the longitudinal displacement is highlighted.     

Characterisation of the reduction properties of La0.5Sr0.5Fe0.5Co0.5O3

We report here on the characterisation by temperature programmed reduction, ⁵⁷Fe Mössbauer spectroscopy and X-ray absorption spectroscopy of the phases resulting from treatment of the perovskite-related material La_0.5Sr_0.5Fe_0.5Co_0.5O₃ in a flowing 90% hydrogen/10% nitrogen atmosphere. The results show that treatment of La_0.5Sr_0.5Fe_0.5Co_0.5O₃ (which contains approximately 50% Fe⁴⁺ and 50% Fe³⁺) in the flowing 90% hydrogen/10% nitrogen atmosphere at 600°C does not result in the reduction of any of the constituent elements of the material and that the perovskite structure is still retained. The Mössbauer spectrum recorded following heating in the gaseous reducing environment at 1,000°C shows the presence of metallic iron, an Fe³⁺-containing phase with parameters compatible with the presence of SrLaFeO₄ which has a K₂NiF₄-type structure, and a paramagnetic Fe³⁺ phase. The X-ray absorption spectroscopy results show the presence of metallic cobalt. The Mössbauer spectrum recorded following heating at 1,200°C continues to show the Fe³⁺-containing components plus a larger contribution from metallic iron. The X-ray absorption spectroscopy results show the presence of metallic cobalt, SrLaFeO₄, La₂O₃ and SrO.     

Non-invasive characterisation of SIX Japanese hand-guards (tsuba)

In this work we present a systematic study of Japanese sword hand-guards (tsuba) carried out by means of non-invasive techniques using neutrons. Several tsuba from different periods, belonging to the Japanese Section of the Stibbert Museum, were analysed using an innovative approach to characterise the bulk of the samples, coupling two neutron techniques, namely Time of Flight Neutron Diffraction (ToF-ND) and Nuclear Resonance Capture Analysis (NRCA). The measurements were carried out on the same instrument: the INES beam-line at the ISIS spallation pulsed neutron source (UK). NRCA analysis allows identifying the elements present in the sample gauge volume, while neutron diffraction is exploited to quantify the phase distribution and other micro-structural parameters of the metal specimen. The results show that all samples are made of high-quality metal, either steel or copper alloy, with noticeable changes in composition and working techniques, depending on the place and time of manufacturing.     

Nonlinear resonant behavior of microbeams over the buckled state

The present study investigates the nonlinear resonant behavior of a microbeam over its buckled (non-trivial) configuration. The system is assumed to be subjected to an axial load along with a distributed transverse harmonic load. The axial load is increased leading the system to lose the stability via a pitchfork bifurcation; the postbuckling configuration is obtained and the nonlinear resonant response of the system over the buckled state is examined. More specifically, the nonlinear equation of motion is obtained employing Hamilton’s principle along with the modified couple stress theory. The continuous system is truncated into a system with finite degrees of freedom; the Galerkin scheme is employed to discretize the nonlinear partial differential equation of motion into a set of ordinary differential equations. This set of equations is solved numerically employing the pseudo-arclength continuation technique; first a nonlinear static analysis is performed upon this set of equations so as to obtain the onset of buckling (supercritical pitchfork bifurcation) and the buckled configuration of the microbeam. The frequency-response and force-response curves of the system are then constructed over the buckled configurations. A comparison is made between the frequency-response curves obtained by means of the modified couple stress and the classical theories. The effect of different system parameters on the frequency-response and force-response curves is also examined.     

The Boltzmann equation from quantum field theory

We show from first principles the emergence of classical Boltzmann equations from relativistic nonequilibrium quantum field theory as described by the Kadanoff–Baym equations. Our method applies to a generic quantum field, coupled to a collection of background fields and sources, in a homogeneous and isotropic spacetime. The analysis is based on analytical solutions to the full Kadanoff–Baym equations, using the WKB approximation. This is in contrast to previous derivations of kinetic equations that rely on similar physical assumptions, but obtain approximate equations of motion from a gradient expansion in momentum space. We show that the system follows a generalized Boltzmann equation whenever the WKB approximation holds. The generalized Boltzmann equation, which includes off-shell transport, is valid far from equilibrium and in a time dependent background, such as the expanding universe.     

Double transverse-spin asymmetries in Drell–Yan processes with antiprotons

We present next-to-leading order predictions for double transverse-spin asymmetries in Drell–Yan dilepton production initiated by proton–antiproton scattering. The kinematic region of the proposed PAX experiment at GSI: 30?s?200 GeV²$30?s?200{\text{GeV}}^2$ and 2?M?7 GeV$2?M?7\text{GeV}$ is examined. The Drell–Yan asymmetries turn out to be large, in the range 20–40%. Measuring these asymmetries would provide the cleanest determination of the quark transversity distributions.     

Enhancing the violation of the einstein-podolsky-rosen local realism by quantum hyperentanglement

Mermin's observation [Phys. Rev. Lett. 65, 1838 (1990)] that the magnitude of the violation of local realism, defined as the ratio between the quantum prediction and the classical bound, can grow exponentially with the size of the system is demonstrated using two-photon hyperentangled states entangled in polarization and path degrees of freedom, and local measurements of polarization and path simultaneously.     

Stochastic acceleration in turbulent electric fields generated by 3D reconnection

Electron and proton acceleration in three-dimensional electric and magnetic fields is studied through test particle simulations. The fields are obtained by a three-dimensional magnetohydrodynamic simulation of magnetic reconnection in slab geometry. The nonlinear evolution of the system is characterized by the growth of many unstable modes and the initial current sheet is fragmented with formation of small scale structures. We inject at random points inside the evolving current sheet a Maxwellian distribution of particles. In a relatively short time (less than a millisecond) the particles develop a power-law tail. The acceleration is extremely efficient and the electrons absorb a large percentage of the available energy in a small fraction of the characteristic time of the MHD simulation, suggesting that resistive MHD codes are unable to represent the full extent of particle acceleration.