Disorder effects in the quantum Heisenberg model: An Extended Dynamical mean-field theory analysis

We investigate a quantum Heisenberg model with both antiferromagnetic and disordered nearest-neighbor couplings. We use an extended dynamical mean-field approach, which reduces the lattice problem to a self-consistent local impurity problem that we solve by using a quantum Monte Carlo algorithm. We consider both two- and three-dimensional antiferromagnetic spin fluctuations and systematically analyze the effect of disorder. We find that in three dimensions for any small amount of disorder a spin-glass phase is realized. In two dimensions, while clean systems display the properties of a highly correlated spin-liquid (where the local spin susceptibility has a non-integer power-low frequency and/or temperature dependence), in the present case this behavior is more elusive unless disorder is very small. This is because the spin-glass transition temperature leaves only an intermediate temperature regime where the system can display the spin-liquid behavior, which turns out to be more apparent in the static than in the dynamical susceptibility.Comment: 15 pages, 7 figure

Spin dynamics of heterometallic Cr7M wheels (M = Mn, Zn, Ni) probed by inelastic neutron scattering

Inelastic neutron scattering has been applied to the study of the spin dynamics of Cr-based antiferromagnetic octanuclear rings where a finite total spin of the ground state is obtained by substituting one Cr(III) ion (s = 3/2) with Zn (s = 0), Mn (s = 5/2) or Ni (s = 1) di-cations. Energy and intensity measurements for several intra-multiplet and inter-multiplet magnetic excitations allow us to determine the spin wavefunctions of the investigated clusters. Effects due to the mixing of different spin multiplets have been considered. Such effects proved to be important to correctly reproduce the energy and intensity of magnetic excitations in the neutron spectra. On the contrary to what is observed for the parent homonuclear Cr8 ring, the symmetry of the first excited spin states is such that anticrossing conditions with the ground state can be realized in the presence of an external magnetic field. Heterometallic Cr7M wheels are therefore good candidates for macroscopic observations of quantum effects.Comment: 9 pages, 11 figures, submitted to Phys. Rev. B, corrected typos and added references, one sentence change

BioWorkbench: A High-Performance Framework for Managing and Analyzing Bioinformatics Experiments

Advances in sequencing techniques have led to exponential growth in biological data, demanding the development of large-scale bioinformatics experiments. Because these experiments are computation- and data-intensive, they require high-performance computing (HPC) techniques and can benefit from specialized technologies such as Scientific Workflow Management Systems (SWfMS) and databases. In this work, we present BioWorkbench, a framework for managing and analyzing bioinformatics experiments. This framework automatically collects provenance data, including both performance data from workflow execution and data from the scientific domain of the workflow application. Provenance data can be analyzed through a web application that abstracts a set of queries to the provenance database, simplifying access to provenance information. We evaluate BioWorkbench using three case studies: SwiftPhylo, a phylogenetic tree assembly workflow; SwiftGECKO, a comparative genomics workflow; and RASflow, a RASopathy analysis workflow. We analyze each workflow from both computational and scientific domain perspectives, by using queries to a provenance and annotation database. Some of these queries are available as a pre-built feature of the BioWorkbench web application. Through the provenance data, we show that the framework is scalable and achieves high-performance, reducing up to 98% of the case studies execution time. We also show how the application of machine learning techniques can enrich the analysis process

White matter integrity as a predictor of response to treatment in first episode psychosis

The integrity of brain white matter connections is central to a patient's ability to respond to pharmacological interventions. This study tested this hypothesis using a specific measure of white matter integrity, and examining its relationship to treatment response using a prospective design in patients within their first episode of psychosis. Diffusion tensor imaging data were acquired in 63 patients with first episode psychosis and 52 healthy control subjects (baseline). Response was assessed after 12 weeks and patients were classified as responders or non-responders according to treatment outcome. At this second time-point, they also underwent a second diffusion tensor imaging scan. Tract-based spatial statistics were used to assess fractional anisotropy as a marker of white matter integrity. At baseline, non-responders showed lower fractional anisotropy than both responders and healthy control subjects (P < 0.05; family-wise error-corrected), mainly in the uncinate, cingulum and corpus callosum, whereas responders were indistinguishable from healthy control subjects. After 12 weeks, there was an increase in fractional anisotropy in both responders and non-responders, positively correlated with antipsychotic exposure. This represents one of the largest, controlled investigations of white matter integrity and response to antipsychotic treatment early in psychosis. These data, together with earlier findings on cortical grey matter, suggest that grey and white matter integrity at the start of treatment is an important moderator of response to antipsychotics. These findings can inform patient stratification to anticipate care needs, and raise the possibility that antipsychotics may restore white matter integrity as part of the therapeutic response

Do observations on surface coverage-reactivity correlations always describe the true catalytic process? A case study on ceria

In situ (operando) investigations aim at establishing structure-function and/or coverage-reactivity correlations. Herein, we investigated the gas-phase HCl oxidation (4HCl + O2 → 2Cl2 + 2H2O) over ceria. Despite its remarkable performance, under low oxygen over-stoichiometry, this oxide is prone to a certain extent to subsurface/bulk chlorination, which leads to deactivation. In situ Prompt Gamma Activation Analysis (PGAA) studies evidenced that the chlorination rate is independent of the pre-chlorination degree but increases at lower oxygen over-stoichiometry, while dechlorination is effective in oxygen-rich feeds, and its rate is higher for a more extensively pre-chlorinated ceria. Even bulk CeCl3 could be transformed into CeO2 under oxygen excess. Electron Paramagnetic Resonance experiments strongly suggested that oxygen activation is inhibited by a high surface chlorination degree. The coverages of most abundant surface intermediates, OH and Cl, were monitored by in situ infrared spectroscopy and PGAA under various conditions. Higher temperature and p(O2) led to enhanced OH coverage, reduced Cl coverage, and increased reactivity. Variation of p(HCl) gave rise to opposite correlations, while raising p(Cl2) did not induce any measurable increase in the Cl coverage, despite the strong inhibition of the reaction rate. The results indicate that only a small fraction of surface sites is actively involved in the reaction, and most of the surface species probed in the in situ observation are spectators. Therefore, when performing in situ steady-state experiments, a large set of variables should be considered to obtain accurate conclusions

Supported CeO₂ catalysts in technical form for sustainable chlorine production

Bulk CeO2 has been recently reported as a promising catalyst for the oxidation of HCl to Cl2. In order to undertake the scale up of this system, various oxides (TiO2, Al2O3 , and low- and high-surface area ZrO2) have been evaluated as carriers. Supported CeO2 catalysts (3–20 wt.% Ce) prepared by dry impregnation were isothermally tested at the lab scale. Their performance was ranked as: CeO2/ZrO2 ≫ CeO2/Al2O3 ≥ CeO2/TiO2. Kinetic data revealed a lower activation energy and a similar activity dependence on the partial pressure of O2 for CeO2/ZrO2 compared to bulk CeO2. Pilot-scale testing over 3-mm pellets of this catalyst evidenced outstanding stability for 700 h on stream. In-depth characterization of the carriers and fresh catalysts by N2 sorption, Hg porosimetry, X-ray diffraction, temperature-programmed reduction with H2, Raman spectroscopy, electron microscopy, and in situ prompt gamma activation analysis, enabled to rationalize the different catalytic behavior of the materials. ZrO2 stabilizes nanostructures of CeO2 and a Ce–Zr mixed oxide phase, which offer high dispersion and improved oxidation properties. The catalyst also shows reduced chlorine uptake, and overall stands as a better Deacon material compared to bulk CeO2 and other supported systems. CeO2 is present on Al2O3 predominantly as well-distributed nanoparticles. Still, alumina does not induce any electronic effect, thus the supported phase behaves similarly to bulk ceria. TiO2, likely due to the structural collapse and dramatic sintering suffered during calcination, leads to the formation of very large ceria particles. Based on our results, CeO2/ZrO2 appears as a robust and cost-effective alternative to the current RuO2-based catalysts for large-scale chlorine recovery

Susceptibility and dilution effects of the kagome bi-layer geometrically frustrated network. A Ga-NMR study of SrCr_(9p)Ga_(12-9p)O_(19)

We present an extensive gallium NMR study of the geometrically frustrated kagome bi-layer compound SrCr_(9p)Ga_(12-9p)O_(19) (Cr^3+, S=3/2) over a broad Cr-concentration range (.72<p<.95). This allows us to probe locally the kagome bi-layer susceptibility and separate the intrinsic properties due to the geometric frustration from those related to the site dilution. Our major findings are: 1) The intrinsic kagome bi-layer susceptibility exhibits a maximum in temperature at 40-50 K and is robust to a dilution as high as ~20%. The maximum reveals the development of short range antiferromagnetic correlations; 2) At low-T, a highly dynamical state induces a strong wipe-out of the NMR intensity, regardless of dilution; 3) The low-T upturn observed in the macroscopic susceptibility is associated to paramagnetic defects which stem from the dilution of the kagome bi-layer. The low-T analysis of the NMR lineshape suggests that the defect can be associated with a staggered spin-response to the vacancies on the kagome bi-layer. This, altogether with the maximum in the kagome bi-layer susceptibility, is very similar to what is observed in most low-dimensional antiferromagnetic correlated systems; 4) The spin glass-like freezing observed at T_g=2-4 K is not driven by the dilution-induced defects.Comment: 19 pages, 19 figures, revised version resubmitted to PRB Minor modifications: Fig.11 and discussion in Sec.V on the NMR shif