Structural Transition Kinetics and Activated Behavior in the Superconducting Vortex Lattice

Using small-angle neutron scattering, we investigated the behavior of a metastable vortex lattice state in MgB2 as it is driven towards equilibrium by an AC magnetic field. This shows an activated behavior, where the AC field amplitude and cycle count are equivalent to, respectively, an effective "temperature" and "time". The activation barrier increases as the metastable state is suppressed, corresponding to an aging of the vortex lattice. Furthermore, we find a cross-over from a partial to a complete suppression of metastable domains depending on the AC field amplitude, which may empirically be described by a single free parameter. This represents a novel kind of collective vortex behavior, most likely governed by the nucleation and growth of equilibrium vortex lattice domains.Comment: 5 pages plus 3 pages of supplemental materia

Topological energy barrier for skyrmion lattice formation in MnSi

We report the direct measurement of the topological skyrmion energy barrier through a hysteresis of the skyrmion lattice in the chiral magnet MnSi. Measurements were made using small-angle neutron scattering with a custom-built resistive coil to allow for high-precision minor hysteresis loops. The experimental data was analyzed using an adapted Preisach model to quantify the energy barrier for skyrmion formation and corroborated by the minimum-energy path analysis based on atomistic spin simulations. We reveal that the skyrmion lattice in MnSi forms from the conical phase progressively in small domains, each of which consisting of hundreds of skyrmions, and with an activation barrier of several eV.Comment: Final accepted versio

Pauli Paramagnetic Effects on Vortices in Superconducting TmNi2B2C

The magnetic field distribution around the vortices in TmNi2B2C in the paramagnetic phase was studied experimentally as well as theoretically. The vortex form factor, measured by small-angle neutron scattering, is found to be field independent up to 0.6 Hc2 followed by a sharp decrease at higher fields. The data are fitted well by solutions to the Eilenberger equations when paramagnetic effects due to the exchange interaction with the localized 4f Tm moments are included. The induced paramagnetic moments around the vortex cores act to maintain the field contrast probed by the form factor.Comment: 4 pages, 4 figure

Observations of Pauli Paramagnetic Effects on the Flux Line Lattice in CeCoIn5

From small-angle neutron scattering studies of the flux line lattice (FLL) in CeCoIn5, with magnetic field applied parallel to the crystal c-axis, we obtain the field- and temperature-dependence of the FLL form factor, which is a measure of the spatial variation of the field in the mixed state. We extend our earlier work [A.D. Bianchi et al. 2008 Science 319, 177] to temperatures up to 1250 mK. Over the entire temperature range, paramagnetism in the flux line cores results in an increase of the form factor with field. Near H_c2 the form factor decreases again, and our results indicate that this fall-off extends outside the proposed FFLO region. Instead, we attribute the decrease to a paramagnetic suppression of Cooper pairing. At higher temperatures, a gradual crossover towards more conventional mixed state behavior is observed.Comment: Submitted to New Journal of Physics, 13 pages, 4 figure

Vortex lattice structure in BaFe2(As0.67P0.33)2 by the small-angle neutron scattering technique

We have observed a magnetic vortex lattice (VL) in BaFe2(As_{0.67}P_{0.33})2 (BFAP) single crystals by small-angle neutron scattering (SANS). With the field along the c-axis, a nearly isotropic hexagonal VL was formed in the field range from 1 to 16 T, which is a record for this technique in the pnictides, and no symmetry changes in the VL were observed. The temperature-dependence of the VL signal was measured and confirms the presence of (non d-wave) nodes in the superconducting gap structure for measurements at 5 T and below. The nodal effects were suppressed at high fields. At low fields, a VL reorientation transition was observed between 1 T and 3 T, with the VL orientation changing by 45{\deg}. Below 1 T, the VL structure was strongly affected by pinning and the diffraction pattern had a fourfold symmetry. We suggest that this (and possibly also the VL reorientation) is due to pinning to defects aligned with the crystal structure, rather than being intrinsic.Comment: 9 pages, 9 figure

Structural studies of metastable and equilibrium vortex lattice domains in MgB2

The vortex lattice in MgB2 is characterized by the presence of long-lived metastable states, which arise from cooling or heating across the equilibrium phase boundaries. A return to the equilibrium configuration can be achieved by inducing vortex motion. Here we report on small-angle neutron scattering studies of MgB2, focusing on the structural properties of the vortex lattice as it is gradually driven from metastable to equilibrium states by an AC magnetic field. Measurements were performed using initial metastable states obtained either by cooling or heating across the equilibrium phase transition. In all cases, the longitudinal correlation length remains constant and comparable to the sample thickness. Correspondingly, the vortex lattice may be considered as a system of straight rods, where the formation and growth of equilibrium state domains only occurs in the two-dimensional plane perpendicular to the applied field direction. Spatially resolved raster scans of the sample were performed with apertures as small as 80 microns, corresponding to only 1.2*10^6 vortices for an applied field of 0.5 T. These revealed spatial variations in the metastable and equilibrium vortex lattice populations, but individual domains were not directly resolved. A statistical analysis of the data indicates an upper limit on the average domain size of approximately 50 microns.Comment: 13 pages, 9 figure

Outer-Sphere Contributions to the Electronic Structure of Type Zero Copper Proteins

Bioinorganic canon states that active-site thiolate coordination promotes rapid electron transfer (ET) to and from type 1 copper proteins. In recent work, we have found that copper ET sites in proteins also can be constructed without thiolate ligation (called “type zero” sites). Here we report multifrequency electron paramagnetic resonance (EPR), magnetic circular dichroism (MCD), and nuclear magnetic resonance (NMR) spectroscopic data together with density functional theory (DFT) and spectroscopy-oriented configuration interaction (SORCI) calculations for type zero Pseudomonas aeruginosa azurin variants. Wild-type (type 1) and type zero copper centers experience virtually identical ligand fields. Moreover, O-donor covalency is enhanced in type zero centers relative that in the C112D (type 2) protein. At the same time, N-donor covalency is reduced in a similar fashion to type 1 centers. QM/MM and SORCI calculations show that the electronic structures of type zero and type 2 are intimately linked to the orientation and coordination mode of the carboxylate ligand, which in turn is influenced by outer-sphere hydrogen bonding

L edge X ray absorption study of mononuclear vanadium complexes and spectral predictions using a restricted open shell configuration interaction ansatz

A series of mononuclear V^(V), V^(IV) and V^(III) complexes were investigated by V L-edge near edge X-ray absorption fine structure (NEXAFS) spectroscopy. The spectra show significant sensitivity to the vanadium oxidation state and the coordination environment surrounding the vanadium center. The L-edge spectra are interpreted with the aid of the recently developed Density Functional Theory/Restricted Open Shell Configuration Interaction Singles (DFT/ROCIS) method. This method is calibrated for the prediction of vanadium L-edges with different hybrid density functionals and basis sets. For the B3LYP/def2-TZVP(-f) and BHLYP/def2-TZVP(-f) functional/basis-set combinations, good to excellent agreement between calculated and experimental spectra is obtained. A treatment of the spin–orbit coupling interaction to all orders is achieved by quasi-degenerate perturbation theory (QDPT), in conjunction with DFT/ROCIS for the calculation of the molecular multiplets while accounting for dynamic correlation and anisotropic covalency. The physical origin of the observed spectral features is discussed qualitatively and quantitatively in terms of spin multiplicities, magnetic sublevels and individual 2p to 3d core level excitations. This investigation is an important prerequisite for future applications of the DFT/ROCIS method to vanadium L-edge absorption spectroscopy and vanadium-based heterogeneous catalysts