Elucidating Individual Magnetic Contributions in Bi-Magnetic Fe3 O4 /Mn3 O4 Core/Shell Nanoparticles by Polarized Powder Neutron Diffraction.

Heterogeneous bi-magnetic nanostructured systems have had a sustained interest during the last decades owing to their unique magnetic properties and the wide range of derived potential applications. However, elucidating the details of their magnetic properties can be rather complex. Here, a comprehensive study of Fe3 O4 /Mn3 O4 core/shell nanoparticles using polarized neutron powder diffraction, which allows disentangling the magnetic contributions of each of the components, is presented. The results show that while at low fields the Fe3 O4 and Mn3 O4 magnetic moments averaged over the unit cell are antiferromagnetically coupled, at high fields, they orient parallel to each other. This magnetic reorientation of the Mn3 O4 shell moments is associated with a gradual evolution with the applied field of the local magnetic susceptibility from anisotropic to isotropic. Additionally, the magnetic coherence length of the Fe3 O4 cores shows some unusual field dependence due to the competition between the antiferromagnetic interface interaction and the Zeeman energies. The results demonstrate the great potential of the quantitative analysis of polarized neutron powder diffraction for the study of complex multiphase magnetic materials.

40-Tesla pulsed-field cryomagnet for single crystal neutron diffraction.

We present the first long-duration and high duty cycle 40-T pulsed-field cryomagnet addressed to single crystal neutron diffraction experiments at temperatures down to 2 K. The magnet produces a horizontal field in a bi-conical geometry, ±15° and ±30° upstream and downstream of the sample, respectively. Using a 1.15 MJ mobile generator, magnetic field pulses of 100 ms length are generated in the magnet, with a rise time of 23 ms and a repetition rate of 6-7 pulses per hour at 40 T. The setup was validated for neutron diffraction on the CEA-CRG three-axis spectrometer IN22 at the Institut Laue Langevin.

Magnetic Fluctuations, Precursor Phenomena, and Phase Transition in MnSi under a Magnetic Field.

The reference chiral helimagnet MnSi is the first system where Skyrmion lattice correlations have been reported. At a zero magnetic field the transition at T_{C} to the helimagnetic state is of first order. Above T_{C}, in a region dominated by precursor phenomena, neutron scattering shows the buildup of strong chiral fluctuating correlations over the surface of a sphere with radius 2π/ℓ, where ℓ is the pitch of the helix. It has been suggested that these fluctuating correlations drive the helical transition to first order following a scenario proposed by Brazovskii for liquid crystals. We present a comprehensive neutron scattering study under magnetic fields, which provides evidence that this is not the case. The sharp first order transition persists for magnetic fields up to 0.4 T whereas the fluctuating correlations weaken and start to concentrate along the field direction already above 0.2 T. Our results thus disconnect the first order nature of the transition from the precursor fluctuating correlations. They also show no indication for a tricritical point, where the first order transition crosses over to second order with increasing magnetic field. In this light, the nature of the first order helical transition and the precursor phenomena above T_{C}, both of general relevance to chiral magnetism, remain an open question.

Implementation of a new Cryopad on the diffractometer POLI at MLZ.

A new polarized neutron single crystal diffractometer POLI (Polarization Investigator) has been developed at the Maier-Leibnitz Zentrum, Garching, Germany. After reviewing existing devices, spherical neutron polarimetry has been implemented on POLI as a main experimental technique using a third-generation cryogenic polarization analysis device (Cryopad) built in cooperation between RWTH University and Institut Laue-Langevin. In this report we describe the realization and present the performance of the new Cryopad on POLI. Some improvements in the construction as well as details regarding calibrations of Cryopad and its practical use are discussed. The reliable operation of the new Cryopad on POLI is also demonstrated.

Field-induced spin-density wave beyond hidden order in URu2Si2.

URu2Si2 is one of the most enigmatic strongly correlated electron systems and offers a fertile testing ground for new concepts in condensed matter science. In spite of >30 years of intense research, no consensus on the order parameter of its low-temperature hidden-order phase exists. A strong magnetic field transforms the hidden order into magnetically ordered phases, whose order parameter has also been defying experimental observation. Here, thanks to neutron diffraction under pulsed magnetic fields up to 40 T, we identify the field-induced phases of URu2Si2 as a spin-density-wave state. The transition to the spin-density wave represents a unique touchstone for understanding the hidden-order phase. An intimate relationship between this magnetic structure, the magnetic fluctuations and the Fermi surface is emphasized, calling for dedicated band-structure calculations.

Chiral paramagnetic skyrmion-like phase in MnSi.

We present a comprehensive study of chiral fluctuations in the reference helimagnet MnSi by polarized neutron scattering and neutron spin echo spectroscopy, which reveals the existence of a completely left-handed and dynamically disordered phase. This phase may be identified as a spontaneous Skyrmion phase: it appears in a limited temperature range just above the helical transition T_{C} and coexists with the helical phase at T_{C}.

Combined charge and spin density experimental study of the yttrium(III) semiquinonato complex Y(HBPz3)2(DTBSQ) and DFT calculations.

High-resolution X-ray diffraction and polarized neutron diffraction experiments have been performed on the Y-semiquinonate complex, Y(HBPz3)2(DTBSQ), in order to determine the charge and spin densities in the paramagnetic ground state, S = (1/2). The aim of these combined studies is to bring new insights to the antiferromagnetic coupling mechanism between the semiquinonate radical and the rare earth ion in the isomorphous Gd(HBPz3)2(DTBSQ) complex. The experimental charge density at 106 K yields detailed information about the bonding between the Y3+ ion and the semiquinonate ligand; the topological charge of the yttrium atom indicates a transfer of about 1.5 electrons from the radical toward the Y3+ ion in the complex, in agreement with DFT calculations. The electron density deformation map reveals well-resolved oxygen lone pairs with one lobe polarized toward the yttrium atom. The determination of the induced spin density at 1.9 K under an applied magnetic field of 9.5 T permits the visualization of the delocalized magnetic orbital of the radical throughout the entire molecule. The spin is mainly distributed on the oxygen atoms [O1 (0.12(1) mu B), O2(0.11(1) mu B)] and the carbon atoms [C21 (0.24(1) mu B), C22(0.20(1) mu B), C24(0.16(1) mu B), C25(0.12(1) mu B)] of the carbonyl ring. A significant spin delocalization on the yttrium site of 0.08(2) mu B is observed, proving that a direct overlap with the radical magnetic orbital can occur at the rare earth site and lead to antiferromagnetic coupling. The DFT calculations are in good quantitative agreement with the experimental charge density results, but they underestimate the spin delocalization of the oxygen toward the yttrium and the carbon atoms of the carbonyl ring.