Magnetic phase diagram of the Hubbard model with next-nearest-neighbour hopping

We calculate the magnetic phase diagram of the Hubbard model for a Bethe lattice with nearest neighbour (NN) hopping $t_1$ and next nearest neighbour (NNN) hopping $t_2$ in the limit of infinite coordination. We use the amplitude $t_2/t_1$ of the NNN hopping to tune the density of states (DOS) of the non-interacting system from a situation with particle-hole symmetry to an asymmetric one with van-Hove singularities at the lower ($t_2/t_1>0$) respectively upper ($t_2/t_1<0$) band edge for large enough $|t_2/t_1|$. For this strongly asymmetric situation we find rather extended parameter regions with ferromagnetic states and regions with antiferromagnetic states.Comment: 13 pages, 7 figure

Interaction between self-excited oscillations and fuel-air mixing in a dual swirl combustor

A partially premixed gas turbine model combustor close to an industrial design is investigated using Large Eddy Simulation (LES). Two flames, one stable and another unstable with self-excited oscillations are computed. In particular, this study addresses the previously unexplained transition of flame shape in the experiments, from V-shaped to flat when the flame becomes acoustically unstable, suggesting a notable change of the important convective delay in the thermoacoustic feedback loop. The LES results show good agreement with the measured velocities, temperature and mass fractions. The acoustic power spectral density (PSD) obtained from the LES of the unstable flame also agrees well with the measured amplitudes in the air plenum and combustion chamber, and reasonably captures the frequency with a slight under-prediction. A comparison of the stable and unstable cases shows different mixing and reaction behaviours despite similar mean velocity fields. Further detailed analysis shows that the different mixing behaviour is driven by the significantly varying air mass split between the two air passages during a thermoacoustic oscillation cycle. This variation is due to the different impedances experienced by the pressure oscillations propagating through the two swirling injector passages with different internal geometries. This causes a periodic variation of the radial momentum of the fuel jets injected between the two swirling air flows. The resulting flapping of the fuel jets creates an enhanced radial fuel-air mixing that leads to a flattened flame in the unstable case. This provides a new physical explanation for the transitions of flame shape observed in the experiments.ZXC and NS acknowledge the support of Mitsubishi Heavy Industries, Japan. This work used the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk) with the computational time provided by the UKCTRF

Multiplet ligand-field theory using Wannier orbitals

We demonstrate how ab initio cluster calculations including the full Coulomb vertex can be done in the basis of the localized, generalized Wannier orbitals which describe the low-energy density functional (LDA) band structure of the infinite crystal, e.g. the transition metal 3d and oxygen 2p orbitals. The spatial extend of our 3d Wannier orbitals (orthonormalized Nth order muffin-tin orbitals) is close to that found for atomic Hartree-Fock orbitals. We define Ligand orbitals as those linear combinations of the O 2p Wannier orbitals which couple to the 3d orbitals for the chosen cluster. The use of ligand orbitals allows for a minimal Hilbert space in multiplet ligand-field theory calculations, thus reducing the computational costs substantially. The result is a fast and simple ab initio theory, which can provide useful information about local properties of correlated insulators. We compare results for NiO, MnO and SrTiO3 with x-ray absorption, inelastic x-ray scattering, and photoemission experiments. The multiplet ligand field theory parameters found by our ab initio method agree within ~10% to known experimental values

The structure of the Au(111)/methylthiolate interface : new insights from near-edge X-ray absorption spectroscopy and X-ray standing waves

The local structure of the Au(111)([square root of]3×[square root of]3)R30°-methylthiolate surface phase has been investigated by S K-edge near-edge s-ray absorption fine structure (NEXAFS) both experimentally and theoretically and by experimental normal-incidence x-ray standing waves (NIXSW) at both the C and S atomic sites. NEXAFS shows not only excitation into the intramolecular sigma* S–C resonance but also into a sigma* S–Au orbital perpendicular to the surface, clearly identifying the local S headgroup site as atop a Au atom. Simulations show that it is not possible, however, to distinguish between the two possible adatom reconstruction models; a single thiolate species atop a hollow-site Au adatom or a dithiolate moiety comprising two thiolate species bonded to a bridge-bonded Au adatom. Within this dithiolate moiety a second sigma* S–Au orbital that lies near parallel to the surface has a higher energy that overlaps that of the sigma* S–C resonance. The new NIXSW data show the S–C bond to be tilted by 61° relative to the surface normal, with a preferred azimuthal orientation in , corresponding to the intermolecular nearest-neighbor directions. This azimuthal orientation is consistent with the thiolate being atop a hollow-site Au adatom, but not consistent with the originally proposed Au-adatom-dithiolate moiety. However, internal conformational changes within this species could, perhaps, render this model also consistent with the experimental data

Self-assembly and two-dimensional spontaneous resolution of cyano-functionalized [7]helicenes on Cu111

Birds of a feather flock together: STM and DFT studies provide the first example of spontaneous chiral resolution of a helicene on a surface. Racemic 6,13-dicyano[7]helicene forms fully segregated domains of pure enantiomers (2D conglomerate) on Cu(111). The propensity of the system to optimize intermolecular CN⋅⋅⋅HC(Ar) hydrogen bonding and CN⋅⋅⋅CN dipolar interactions translates into chiral recognition with preferential assembly of homochiral molecules

Atomic and itinerant effects at the transition metal x-ray absorption K-pre-edge exemplified in the case of V2_2O3_3

X-ray absorption spectroscopy is a well established tool for obtaining information about orbital and spin degrees of freedom in transition metal- and rare earth-compounds. For this purpose usually the dipole transitions of the L- (2p to 3d) and M- (3d to 4f) edges are employed, whereas higher order transitions such as quadrupolar 1s to 3d in the K-edge are rarely studied in that respect. This is due to the fact that usually such quadrupolar transitions are overshadowed by dipole allowed 1s to 4p transitions and, hence, are visible only as minor features in the pre-edge region. Nonetheless, these features carry a lot of valuable information, similar to the dipole L-edge transition, which is not accessible in experiments under pressure due to the absorption of the diamond anvil pressurecell. We recently performed a theoretical and experimental analysis of such a situation for the metal insulator transition of (V(1-x)Crx)2O3. Since the importance of the orbital degrees of freedom in this transition is widely accepted, a thorough understanding of quadrupole transitions of the vanadium K-pre-edge provides crucial information about the underlying physics. Moreover, the lack of inversion symetry at the vanadium site leads to onsite mixing of vanadium 3d- and 4p- states and related quantum mechanical interferences between dipole and quadrupole transitions. Here we present a theoretical analysis of experimental high resolution x-ray absorption spectroscopy at the V pre-K edge measured in partial fluorescence yield mode for single crystals. We carried out density functional as well as configuration interaction calculations in order to capture effects coming from both, itinerant and atomic limits

Magnetic versus crystal field linear dichroism in NiO thin films

We have detected strong dichroism in the Ni $L_{2,3}$ x-ray absorption spectra of monolayer NiO films. The dichroic signal appears to be very similar to the magnetic linear dichroism observed for thicker antiferromagnetic NiO films. A detailed experimental and theoretical analysis reveals, however, that the dichroism is caused by crystal field effects in the monolayer films, which is a non trivial effect because the high spin Ni $3d^{8}$ ground state is not split by low symmetry crystal fields. We present a practical experimental method for identifying the independent magnetic and crystal field contributions to the linear dichroic signal in spectra of NiO films with arbitrary thicknesses and lattice strains. Our findings are also directly relevant for high spin $3d^{5}$ and $3d^{3}$ systems such as LaFeO$_{3}$, Fe$_{2}$O$_{3}$, VO, LaCrO$_{3}$, Cr$_{2}$O$_{3}$, and Mn$^{4+}$ manganate thin films

Large Eddy Simulation of a dual swirl gas turbine combustor: Flame/flow structures and stabilisation under thermoacoustically stable and unstable conditions

A laboratory gas turbine model combustor with dual-swirler configuration is in- vestigated using Large Eddy Simulation (LES) with a flamelet subgrid combus- tion model. Two partially premixed methane/air flames with different equivalence ratio and thermal power are simulated: one stably burning with an elongated V- shape and another undergoing pronounced thermoacoustic oscillations exhibiting a flat shape. Additionally, both flames feature a hydrodynamic instability in the form of a precessing vortex core (PVC). Detailed comparisons between experi- mental and LES results show that the different flow and reaction zone structures in these two flames are reproduced well. The various flow dynamics resulting from the PVC and thermoacoustic oscillations are also captured accurately in the simulation. Further analyses on the lifted swirl flame stabilisation using phase averaged statistics at the PVC frequencies reveal that the PVC-induced stagnation points provide an anchoring mechanism for both the stable and unstable flames, although in the latter case large self-excited pressure oscillations are present. It is found that the PVC is significantly influenced by these oscillations, being axially stretched and compressed at high and low pressures, respectively. However, the formation of flame leading edge due to the PVC is robust during these unstable processes and the azimuthal movement of the leading point is found to be strongly correlated with the rotation of the PVC in both flames, further confirming the vital role of the PVC in the stabilisation process of these lifted swirl flames

Three-dimensional magnetic flux-closure patterns in mesoscopic Fe islands

We have investigated three-dimensional magnetization structures in numerous mesoscopic Fe/Mo(110) islands by means of x-ray magnetic circular dichroism combined with photoemission electron microscopy (XMCD-PEEM). The particles are epitaxial islands with an elongated hexagonal shape with length of up to 2.5 micrometer and thickness of up to 250 nm. The XMCD-PEEM studies reveal asymmetric magnetization distributions at the surface of these particles. Micromagnetic simulations are in excellent agreement with the observed magnetic structures and provide information on the internal structure of the magnetization which is not accessible in the experiment. It is shown that the magnetization is influenced mostly by the particle size and thickness rather than by the details of its shape. Hence, these hexagonal samples can be regarded as model systems for the study of the magnetization in thick, mesoscopic ferromagnets.Comment: 12 pages, 11 figure

Stepwise Adsorption of Alkoxy-Pyrene Derivatives onto a Lamellar, Non-Porous Naphthalenediimide-Template on HOPG

The development of new strategies for the preparation of multicomponent supramolecular assemblies is a major challenge on the road to complex functional molecular systems. Here we present the use of a non-porous self-assembled monolayer from uC33-NDI-uC33, a naphthalenediimide symmetrically functionalized with unsaturated 33 carbon-atom-chains, to prepare bicomponent supramolecular surface systems with a series of alkoxy-pyrene (PyrOR) derivatives at the liquid/HOPG interface. While previous attempts at directly depositing many of these PyrOR units at the liquid/HOPG interface failed, the multicomponent approach through the uC33-NDI-uC33 template enabled control over molecular interactions and facilitated adsorption. The PyrOR deposition restructured the initial uC33-NDI-uC33 monolayer, causing an expansion in two dimensions to accommodate the guests. As far as we know, this represents the first example of a non-porous or non-metal complex-bearing monolayer that allows the stepwise formation of multicomponent supramolecular architectures on surfaces