Saman Ghannadzadeh

Evolution Of Magnetic Interactions In A Pressure-Induced Jahn-Teller Driven Magnetic Dimensionality Switch

We present the results of high-field magnetization and muon-spin relaxation measurements on the coordination polymer CuF 2 (H 2 O) 2 (pyrazine) in pressures up to 22.5 kbar. We observe a transition from a quasi-two-dimensional to a quasi-one-dimensional antiferromagnetic phase at 9.1 kbar, driven by a rotation of the Jahn-Teller axis. Long-range antiferromagnetic ordering is seen in both regimes, as well as a phase separation in the critical pressure region. The magnetic dimensionality switching as pressure is increased is accompanied by a halving of the primary magnetic exchange energy J and a fivefold decrease in the ordering temperature T N . J decreases gradually with pressure in the two-dimensional phase, and then increases in the one-dimensional regime. We relate both effects to the changes in the crystal structure with applied pressure.

Influence of HF2- geometry on magnetic interactions elucidated from polymorphs of the metal-organic framework [Ni(HF2)(pyz)2]PF6 (pyz = pyrazine).

A tetragonal polymorph of [Ni(HF(2))(pyz)(2)]PF(6) (designated β) is isomorphic to its SbF(6)-congener at 295 K and features linear Ni-FHF-Ni pillars. Enhancements in the spin exchange (J(FHF) = 7.7 K), Néel temperature (T(N) = 7 K), and critical field (B(c) = 24 T) were found relative to monoclinic α-PF(6). DFT reveals that the HF(2)(-) bridges are significantly better mediators of magnetic exchange than pyz (J(pyz)), where J(FHF) ≈ 3J(pyz), thus leading to quasi-1D behavior. Spin density resides on all atoms of the HF(2)(-) bridge whereas N-donor atoms of the pyz ring bear most of the density.

Low-moment magnetism in the double perovskites Ba2M OsO6 (M =Li,Na)

The magnetic ground states of the isostructural double perovskites Ba2NaOsO6 and Ba2LiOsO6 are investigated with muon-spin rotation. In Ba2NaOsO6 long-range magnetic order is detected via the onset of a spontaneous muon-spin precession signal below Tc = 7.2±0.2 K, while in Ba2LiOsO6 a static but spatially-disordered internal field is found below 8 K. A novel probabilistic argument is used to show from the observed precession frequencies that the magnetic ground state in Ba2NaOsO6 is most likely to be low-moment (� 0.2µB) ferromagnetism and not canted antiferromagnetism. Ba2LiOsO6 is antiferromagnetic and we find a spin-flop transition at 5.5T. A reduced osmium moment is common to both compounds, probably arising from a combination of spin-orbit coupling and frustration.

[Ni(HF2)(3-Clpy)4]BF4 (py = pyridine): evidence for spin exchange along strongly distorted F···H···F- bridges in a one-dimensional polymeric chain.

[Ni(HF(2))(3-Clpy)(4)]BF(4) (py = pyridine) is a simple one-dimensional (1D) coordination polymer composed of compressed NiN(4)F(2) octahedra that form chains with bridging HF(2)(-) ligands. In spite of significant distortion of the HF(2)(-) bridge, a quasi-1D antiferromagnetic (AFM) behavior was observed with J(FHF) = 4.86 K.

Measurement of magnetic susceptibility in pulsed magnetic fields using a proximity detector oscillator

We present a novel susceptometer with a particularly small spatial footprint and no moving parts. The susceptometer is suitable for use in systems with limited space where magnetic measurements may not have been previously possible, such as in pressure cells and rotators, as well as in extremely high pulsed fields. The susceptometer is based on the proximity detector oscillator, which has a broad dynamic resonant frequency range and has so far been used predominantly for transport measurements. We show that for insulating samples, the resonance frequency behavior as a function of field consists of a magnetoresistive and an inductive component, originating, respectively, from the sensor coil and the sample. The response of the coil is modeled, and upon subtraction of the magnetoresistive component the dynamic magnetic susceptibility and magnetization can be extracted. We successfully measure the magnetization of the organic molecular magnets Cu(H(2)O)(5)(VOF(4))(H(2)O) and [Cu(HF(2))(pyz)(2)]BF(4) in pulsed magnetic fields and by comparing the results to that from a traditional extraction susceptometer confirm that the new system can be used to measure and observe magnetic susceptibilities and phase transitions.

Antiferromagnetism in a Family of S = 1 Square Lattice Coordination Polymers NiX2(pyz)2 (X = Cl, Br, I, NCS; pyz = Pyrazine)

The crystal structures of NiX2(pyz)2 (X = Cl (1), Br (2), I (3), and NCS (4)) were determined by synchrotron X-ray powder diffraction. All four compounds consist of two-dimensional (2D) square arrays self-assembled from octahedral NiN4X2 units that are bridged by pyz ligands. The 2D layered motifs displayed by 1-4 are relevant to bifluoride-bridged [Ni(HF2)(pyz)2]EF6 (E = P, Sb), which also possess the same 2D layers. In contrast, terminal X ligands occupy axial positions in 1-4 and cause a staggered packing of adjacent layers. Long-range antiferromagnetic (AFM) order occurs below 1.5 (Cl), 1.9 (Br and NCS), and 2.5 K (I) as determined by heat capacity and muon-spin relaxation. The single-ion anisotropy and g factor of 2, 3, and 4 were measured by electron-spin resonance with no evidence for zero-field splitting (ZFS) being observed. The magnetism of 1-4 spans the spectrum from quasi-two-dimensional (2D) to three-dimensional (3D) antiferromagnetism. Nearly identical results and thermodynamic features were obtained for 2 and 4 as shown by pulsed-field magnetization, magnetic susceptibility, as well as their Néel temperatures. Magnetization curves for 2 and 4 calculated by quantum Monte Carlo simulation also show excellent agreement with the pulsed-field data. Compound 3 is characterized as a 3D AFM with the interlayer interaction (J⊥) being slightly stronger than the intralayer interaction along Ni-pyz-Ni segments (J(pyz)) within the two-dimensional [Ni(pyz)2](2+) square planes. Regardless of X, J(pyz) is similar for the four compounds and is roughly 1 K.

Robustness of superconductivity to structural disorder in Sr

The superconducting properties of a recently discovered high-Tc superconductor, Sr/ammonia-intercalated FeSe, have been measured using pulsed magnetic fields down to 4.2 K and muon spin spectroscopy down to 1.5 K. This compound exhibits intrinsic disorder resulting from random stacking of the FeSe layers along the c axis that is not present in other intercalates of the same family. This arises because the coordination requirements of the intercalated Sr and ammonia moieties imply that the interlayer stacking (along c) involves a translation of either a/2 or b/2 that locally breaks tetragonal symmetry. The result of this stacking arrangement is that the Fe ions in this compound describe a body-centered-tetragonal lattice in contrast to the primitive arrangement of Fe ions described in all other Fe-based superconductors. In pulsed magnetic fields, the upper critical field Hc2 was found to increase on cooling with an upward curvature that is commonly seen in type-II superconductors of a multiband nature. Fitting the data to a two-band model and extrapolation to absolute zero gave a maximum upper critical field μ0Hc2(0) of 33(2)T. A clear superconducting transition with a diamagnetic shift was also observed in transverse-field muon measurements at Tc≈36.3(2)K. These results demonstrate that robust superconductivity in these intercalated FeSe systems does not rely on perfect structural coherence along the c axis.

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We investigate the structural and magnetic properties of two molecule-based magnets synthesized from the same starting components. Their different structural motifs promote contrasting exchange pathways and consequently lead to markedly different magnetic ground states. Through examination of their structural and magnetic properties we show that [Cu(pyz)(H 2 O)(gly) 2 ](ClO 4 ) 2 may be considered a quasi-one-dimensional quantum Heisenberg antiferromagnet whereas the related compound [Cu(pyz)(gly)](ClO 4 ) , which is formed from dimers of antiferromagnetically interacting Cu 2+ spins, remains disordered down to at least 0.03 K in zero field but shows a field-temperature phase diagram reminiscent of that seen in materials showing a Bose-Einstein condensation of magnons.

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Strong hydrogen bonds such as F···H···F offer new strategies to fabricate molecular architectures exhibiting novel structures and properties. Along these lines and, to potentially realize hydrogen-bond mediated superexchange interactions in a frustrated material, we synthesized [H2F]2[Ni3F6(Fpy)12][SbF6]2 (Fpy = 3-fluoropyridine). It was found that positionally-disordered H2F+ ions link neutral NiF2(Fpy)4 moieties into a kagome lattice with perfect 3-fold rotational symmetry. Detailed magnetic investigations combined with density-functional theory (DFT) revealed weak antiferromagnetic interactions (J ~ 0.4 K) and a large positive-D of 8.3 K with ms = 0 lying below ms = ±1. The observed weak magnetic coupling is attributed to bond-disorder of the H2F+ ions which leads to disrupted Ni-F···H-F-H···F-Ni exchange pathways. Despite this result, we argue that networks such as this may be a way forward in designing tunable materials with varying degrees of frustration.

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The upper critical field of NaFe1−xCoxAs was measured from x=0 to x=0.08, with the magnetic field applied parallel (H∥c2) and normal (H⊥c2) to the planes. The data were fitted using one-band and two-band models. The orbital and paramagnetic components of the upper critical field were extracted for H∥c2, which we find to be strongly dominated by paramagnetic pair breaking. In the parent compound the paramagnetic limit is equal to the value expected by BCS theory. However, substitution of Fe by Co leads to an enhancement above the BCS limit by a factor of approximately 1.6. In the overdoped region, we observe a significant convex curvature in H⊥c2 at low temperatures, which we attribute to the two-band nature of the superconductivity and the asymmetry between the two bands. Additionally, we discuss the behavior of critical field anisotropy, coherence length ξ, and the penetration depth λ.