Relativistic laser channeling in plasmas for fast ignition

We report an experimental observation suggesting plasma channel formation by focusing a relativistic laser pulse into a long-scale-length preformed plasma. The channel direction coincides with the laser axis. Laser light transmittance measurement indicates laser channeling into the high-density plasma with relativistic self-focusing. A three-dimensional particle-in-cell simulation reproduces the plasma channel and reveals that the collimated hot-electron beam is generated along the laser axis in the laser channeling. These findings hold the promising possibility of fast heating a dense fuel plasma with a relativistic laser pulse.

Quantum Mechanics Studies of Fuel Cell Catalysts and Proton Conducting Ceramics with Validation by Experiment

We carried out quantum mechanics (QM) studies aimed at improving the performance of hydrogen fuel cells. This led to predictions of improved materials, some of which were subsequently validated with experiments by our collaborators.

In part I, the challenge was to find a replacement for the Pt cathode that would lead to improved performance for the Oxygen Reduction Reaction (ORR) while remaining stable under operational conditions and decreasing cost. Our design strategy was to find an alloy with composition Pt3M that would lead to surface segregation such that the top layer would be pure Pt, with the second and subsequent layers richer in M. Under operating conditions we expect the surface to have significant O and/or OH chemisorbed on the surface, and hence we searched for M that would remain segregated under these conditions. Using QM we examined surface segregation for 28 Pt₃M alloys, where M is a transition metal. We found that only Pt₃Os and Pt₃Ir showed significant surface segregation when O and OH are chemisorbed on the catalyst surfaces. This result indicates that Pt₃Os and Pt3Ir favor formation of a Pt-skin surface layer structure that would resist the acidic electrolyte corrosion during fuel cell operation environments. We chose to focus on Os because the phase diagram for Pt-Ir indicated that Pt-Ir could not form a homogeneous alloy at lower temperature. To determine the performance for ORR, we used QM to examine all intermediates, reaction pathways, and reaction barriers involved in the processes for which protons from the anode reactions react with O₂ to form H₂O. These QM calculations used our Poisson-Boltzmann implicit solvation model include the effects of the solvent (water with dielectric constant 78 with pH 7 at 298K). We found that the rate determination step (RDS) was the O_ad hydration reaction (O_ad + H₂O_ad -> OH_ad + OH_ad) in both cases, but that the barrier for pure Pt of 0.50 eV is reduced to 0.48 eV for Pt₃Os, which at 80 degrees C would increase the rate by 218%. We collaborated with the Pu-Wei Wu’s group to carry out experiments, where we found that the dealloying process-treated Pt2Os catalyst showed two-fold higher activity at 25 degrees C than pure Pt and that the alloy had 272% improved stability, validating our theoretical predictions.

We also carried out similar QM studies followed by experimental validation for the Os/Pt core-shell catalyst fabricated by the underpotential deposition (UPD) method. The QM results indicated that the RDS for ORR is a compromise between the OOH formation step (0.37 eV for Pt, 0.23 eV for Pt_2ML/Os core-shell) and H₂O formation steps (0.32 eV for Pt, 0.22 eV for Pt_2ML/Os core-shell). We found that Pt_2ML/Os has the highest activity (compared to pure Pt and to the Pt₃Os alloy) because the 0.37 eV barrier decreases to 0.23 eV. To understand what aspects of the core shell structure lead to this improved performance, we considered the effect on ORR of compressing the alloy slab to the dimensions of pure Pt. However this had little effect, with the same RDS barrier 0.37 eV. This shows that the ligand effect (the electronic structure modification resulting from the Os substrate) plays a more important role than the strain effect, and is responsible for the improved activity of the core- shell catalyst. Experimental materials characterization proves the core-shell feature of our catalyst. The electrochemical experiment for Pt_2ML/Os/C showed 3.5 to 5 times better ORR activity at 0.9V (vs. NHE) in 0.1M HClO₄ solution at 25 degrees C as compared to those of commercially available Pt/C. The excellent correlation between experimental half potential and the OH binding energies and RDS barriers validate the feasibility of predicting catalyst activity using QM calculation and a simple Langmuir–Hinshelwood model.

In part II, we used QM calculations to study methane stream reforming on a Ni-alloy catalyst surfaces for solid oxide fuel cell (SOFC) application. SOFC has wide fuel adaptability but the coking and sulfur poisoning will reduce its stability. Experimental results suggested that the Ni4Fe alloy improves both its activity and stability compared to pure Ni. To understand the atomistic origin of this, we carried out QM calculations on surface segregation and found that the most stable configuration for Ni₄Fe has a Fe atom distribution of (0%, 50%, 25%, 25%, 0%) starting at the bottom layer. We calculated that the binding of C atoms on the Ni4Fe surface is 142.9 Kcal/mol, which is about 10 Kcal/mol weaker compared to the pure Ni surface. This weaker C binding energy is expected to make coke formation less favorable, explaining why Ni₄Fe has better coking resistance. This result confirms the experimental observation. The reaction energy barriers for CHx decomposition and C binding on various alloy surface, Ni₄X (X=Fe, Co, Mn, and Mo), showed Ni₄Fe, Ni₄Co, and Fe₄Mn all have better coking resistance than pure Ni, but that only Ni₄Fe and Fe₄Mn have (slightly) improved activity compared to pure Ni.

In part III, we used QM to examine the proton transport in doped perovskite-ceramics. Here we used a 2x2x2 supercell of perovskite with composition Ba₈X₇M₁(OH)₁O₂₃ where X=Ce or Zr and M=Y, Gd, or Dy. Thus in each case a 4⁺ X is replace by a 3⁺ M plus a proton on one O. Here we predicted the barriers for proton diffusion allowing both includes intra-octahedron and inter-octahedra proton transfer. Without any restriction, we only observed the inter-octahedra proton transfer with similar energy barrier as previous computational work but 0.2 eV higher than experimental result for Y doped zirconate. For one restriction in our calculations is that the O_donor-O_acceptor atoms were kept at fixed distances, we found that the barrier difference between cerates/zirconates with various dopants are only 0.02~0.03 eV. To fully address performance one would need to examine proton transfer at grain boundaries, which will require larger scale ReaxFF reactive dynamics for systems with millions of atoms. The QM calculations used here will be used to train the ReaxFF force field.

I. Anisotropy and crystal structure of ferromagnetic thin films. II. Investigations into magnetic microstructure by Lorentz microscopy

The induced magnetic uniaxial anisotropy of Ni-Fe alloy films has been shown to be related to the crystal structure of the film. By use of electron diffraction, the crystal structure or vacuum-deposited films was determined over the composition range 5% to 85% Ni, with substrate temperature during deposition at various temperatures in the range 25° to 500° C. The phase diagram determined in this way has boundaries which are in fair agreement with the equilibrium boundaries for bulk material above 400°C. The (α+ ɤ) mixture phase disappears below 100°C.

The measurement of uniaxial anisotropy field for 25% Ni-Fe alloy films deposited at temperatures in the range -80°C to 375°C has been carried out. Comparison of the crystal structure phase diagram with the present data and those published by Wilts indicates that the anisotropy is strongly sensitive to crystal structure. Others have proposed pair ordering as an important source of anisotropy because of an apparent peak in the anisotropy energy at about 50% Ni composition. The present work shows no such peak, and leads to the conclusion that pair ordering cannot be a dominant contributor.

Width of the 180° domain wall in 76% Ni-Fe alloy films as a function of film thickness up to 1800 Å was measured using the defocused mode of Lorentz microscopy. For the thinner films, the measured wall widths are in good agreement with earlier data obtained by Fuchs. For films thicker than 800 Å, the wall width increases with film thickness to about 9000 Å at 1800 Å film thickness. Similar measurements for polycrystalline Co films with thickness from 200 to 1500 Å have been made. The wall width increases from 3000 Å at 400 Å film thickness to about 6000 Å at 1500 Å film thickness. The wall widths for Ni-Fe and Co films are much greater than predicted by present theories. The validity of the classical determination of wall width is discussed, and the comparison of the present data with theoretical results is given.

Finally, an experimental study of ripple by Lorentz microscopy in Ni-Fe alloy films has been carried out. The following should be noted: (1) the only practical way to determine experimentally a meaningful wavelength is to find a well-defined ripple periodicity by visual inspection of a photomicrograph. (2) The average wavelength is of the order of 1µ. This value is in reasonable agreement with the main wavelength predicted by the theories developed by others. The dependence of wavelength on substrate deposition temperature, alloy composition and the external magnetic field has been also studied and the results are compared with theoretical predictions. (3) The experimental fact that the ripple structure could not be observed in completely epitaxial films gives confirmation that the ripple results from the randomness of crystallite orientation. Furthermore, the experimental observation that the ripple disappeared in the range 71 and 75% Ni supports the theory that the ripple amplitude is directly dependent on the crystalline anisotropy. An attempt to experimentally determine the order of magnitude of the ripple angle was carried out. The measured angle was about 0.02 rad. The discrepancy between the experimental data and the theoretical prediction is serious. The accurate experimental determination of ripple angle is an unsolved problem.

Transverse mode formation in longitudinally pumped miniature slab lasers

The formation of transverse modes in longitudinally pumped miniature slab lasers is investigated theoretically and experimentally. The longitudinally non-uniform gain-guiding is studied by expanding the electric field into the Hermite-Gaussian functions that satisfy boundary conditions of the resonator. Non-Gaussian transversal beam profiles in the near field are found and the beam diameter is reduced when the pump spot becomes smaller. The experimental observation agrees with the theoretical calculation.

Mode competition in acousto-optically Q-switched planar waveguide lasers

Multi-mode rate equations have been developed to investigate mode competition in high-power acousto-optically Q-switched planar waveguide lasers. The mode competition arises from coupling effects and temporal losses in the transform between guided modes and free-space propagation. Pulse-to-pulse instability and temporal beam distortions are enlarged by mode competition when the laser works in the multi-mode regime. The influence of parasitic oscillation is also discussed. A Nd:YAG planar waveguide laser has been established with a folded hybrid/unstable resonator. A maximum average power of 83 W with a beam propagation factor M-x(2) x M-y(2) = 1.2 x 1.4 is obtained. The theoretical simulation agrees well with the experimental observation. (c) 2006 Elsevier Ltd. All rights reserved.

Investigation of air-core vortex at hydraulic intakes

Hydrodynamic properties of the surface vortex have been investigated. Based on the Navier-Stokes equations, three sets of the new formulations for the tangential velocity distributions are derived, and verified against the experimental measurements in the literature. It is shown that one modification greatly improves the agreement with the experimental data. Physical model experiments were carried out to study the intake vortex related to the Xiluodu hydropower project. The velocity fields were measured using the Particle Tracking Velocimetry (PTV) technique. The proposed equation for tangential velocity distribution is applied to the Xiluodu project with the solid boundary being considered by the method of images. Good agreement has been observed between the formula prediction and the experimental observation. © 2010 Publishing House for Journal of Hydrodynamics.

Bypass transition to sustained thermoacoustic oscillations in a linearly stable rijke tube

In this paper we examine triggering in a simple linearly-stable thermoacoustic system using techniques from flow instability and optimal control. Firstly, for a noiseless system, we find the initial states that have highest energy growth over given times and from given energies. Secondly, by varying the initial energy, we find the lowest energy that just triggers to a stable periodic solution. We show that the corresponding initial state grows first towards an unstable periodic solution and, from there, to the stable periodic solution. This exploits linear transient growth, which arises due to nonnormality in the governing equations and is directly analogous to bypass transition to turbulence. Thirdly, we introduce noise that has similar spectral characteristics to this initial state. We show that, when triggering from low noise levels, the system grows to high amplitude self-sustained oscillations by first growing towards the unstable periodic solution of the noiseless system. This helps to explain the experimental observation that linearly-stable systems can trigger to self-sustained oscillations even with low background noise. © 2010 by University of Cambridge. Published by the American Institute of Aeronautics and Astronautics, Inc.

Confined LO-phonon-assisted magnetotunneling in a parabolic quantum well with double barriers

The confined longitudinal-optical phonon-assisted tunneling through a parabolic quantum well with double barriers in a magnetic field perpendicular to the interfaces is studied theoretically based on a dielectric continuum model. The numerical results show that the applied magnetic field sharpens and heightens the phonon-assisted tunneling peaks in agreement with experimental observation. Furthermore, the phonon-assisted magnetotunneling peaks shift towards the higher biases as the magnetic field increases. In contrast to the results for a rectangular quantum well, the ratio of peak to valley of the phonon-assisted tunneling is larger for the wider well case. It also indicates that the phonon-assisted tunneling current peaks can be easily observed for a wider parabolic quantum well. (C) 2008 Published by Elsevier B.V.

Effect of defects on optical phonon Raman spectra in SiC nanorods

Fabricated one-dimensional (1D) materials often have abundant structural defects. Experimental observation and numerical calculation indicate that the broken translation symmetry due to structural defects may play a more important role than the quantum confinement effect in the Raman features of optical phonons in polar semiconductor quantum wires such as SiC nanorods, (C) 1999 Elsevier Science Ltd. All rights reserved.

Two-dimensional photovoltaic dark spatial solitons of partially spatially incoherent light

We report a successful experimental observation of two-dimensional photovoltaic dark solitons in an anisotropic crystal with partially spatially incoherent light beams. This kind of solitons results from the bulk photovoltaic effect, which depends on the direction of propagation of the optical beam and on the orientation of the intensity gradient, with respect to the principal axes of the crystal.

Perpendicular-electric-field dependence of exciton binding energy studied by continuous-wave photoluminescence

The reduction of exciton binding energy induced by a perpendicular electric field in a stepped quantum well is studied. From continuous-wave photoluminescence spectra at 77 K we have observed an obvious blueshift of the exciton peak due to a spatially direct-to-indirect transition of excitons. A simple method is used to calculate the exciton binding energy while the inhomogeneous broadening is taken into account in a simple manner. The calculated result reproduces remarkably well the experimental observation.

Role of the N

New measurement by CELSIUS-WASA Collaboration on the pp →pnπ+ reaction reveals clear evidence for the presence of the Roper resonance N∗(1440) which has been ignored in previous theoretical calculations. In this article, based on an effective Lagrangian approach and available knowledge on the Roper resonance, we investigate the role of the Roper resonance for the pp→pnπ+ reaction. It is found that the contribution from the Roper resonance N∗(1440) becomes significant for kinetic energy above 1.1 GeV, consistent with the new experimental observation. The t -channel σ-meson exchange is dominant for the production of the Roper resonance.

Kondo Effect in Carbon Nanotube Quantum Dots with Spin-Orbit Coupling

Motivated by recent experimental observation of spin-orbit coupling in carbon nanotube quantum dots [F. Kuemmeth , Nature (London) 452, 448 (2008)], we investigate in detail its influence on the Kondo effect. The spin-orbit coupling intrinsically lifts out the fourfold degeneracy of a single electron in the dot, thereby breaking the SU(4) symmetry and splitting the Kondo resonance even at zero magnetic field. When the field is applied, the Kondo resonance further splits and exhibits fine multipeak structures resulting from the interplay of spin-orbit coupling and the Zeeman effect. A microscopic cotunneling process for each peak can be uniquely identified. Finally, a purely orbital Kondo effect in the two-electron regime is also predicted.

Low-spin signature inversion in the pi h(9/2)circle times nu i(13/2) oblate band

Excited states in Tl-188,Tl-190 have been studied experimentally by means of in-beam gamma spectroscopy techniques, and resulted in the identification of a strongly coupled band based on the pi h(9/2) circle times nu i(13/2) configuration with oblate deformation. The oblate band in doubly odd Tl nuclei shows low-spin signature inversion. It is the first experimental observation of low-spin signature inversion for a band associated with the oblate pi h(9/2) circle times nu i(13/2) configuration.

Ab initio study on the electronic, magnetic, and mechanical properties of CaCu3V4O12

The electronic, magnetic, and mechanical properties of CaCu3V4O12 are investigated by use of the density functional theory method. The calculated results indicate that CaCu3V4O12 is a half-metallic and ferrimagnetic compound. The magnetic coupling for Cu-V is antiferromagnetic, while those for Cu-Cu and V-V are ferromagnetic. The obtained elastic constants suggest that the compound is mechanically stable. The calculated oxidation states and density of states reveal the existence of a mixed valence for Cu and V. This supports the experimental observation of the mixed valence in Ca2+Cu2+Cu2+(V25+V24+)O-12.