Daniel Haskel

Hyperhoneycomb Iridate β − Li 2 IrO 3 as a Platform for Kitaev Magnetism

A complex iridium oxide β-Li(2)IrO(3) crystallizes in a hyperhoneycomb structure, a three-dimensional analogue of honeycomb lattice, and is found to be a spin-orbital Mott insulator with J(eff)=1/2 moment. Ir ions are connected to the three neighboring Ir ions via Ir-O(2)-Ir bonding planes, which very likely gives rise to bond-dependent ferromagnetic interactions between the J(eff)=1/2 moments, an essential ingredient of Kitaev model with a spin liquid ground state. Dominant ferromagnetic interaction between J(eff)=1/2 moments is indeed confirmed by the temperature dependence of magnetic susceptibility χ(T) which shows a positive Curie-Weiss temperature θ(CW)∼+40  K. A magnetic ordering with a very small entropy change, likely associated with a noncollinear arrangement of J(eff)=1/2 moments, is observed at T(c)=38  K. With the application of magnetic field to the ordered state, a large moment of more than 0.35  μ(B)/Ir is induced above 3 T, a substantially polarized J(eff)=1/2 state. We argue that the close proximity to ferromagnetism and the presence of large fluctuations evidence that the ground state of hyperhoneycomb β-Li(2)IrO(3) is located in close proximity of a Kitaev spin liquid.

Electronic structure and magnetism in compressed 3d transition metals

The authors present a systematic study of high-pressure effects on electronic structure and magnetism in 3d transition metals (Fe, Co, and Ni) based on x-ray magnetic circular dichroism measurements. The data show that the net magnetic moment in Fe vanishes above 18GPa upon the transition to hcp Fe, while both cobalt and nickel remain ferromagnetic to well over 100GPa. The authors estimate the total disappearance of moment in hcp Co at around 150GPa and predict a nonmagnetic Ni phase above 250GPa. The present data suggest that the suppression of ferromagnetism in Fe, Co, and Ni is due to pressure-induced broadening of the 3d valence bands.

A new approach for improving exchange-spring magnets

It is demonstrated here that an already ideal exchange–spring magnet can be further improved by intermixing the interface. This is counter-intuitive to the general expectation that optimal exchange–spring magnet behavior requires an ideal, atomically coherent soft–hard interface. Epitaxial Sm–Co/Fe thin-film exchange–spring bilayers are thermally processed, by annealing or high-temperature deposition, to induce interdiffusion. With increasing processing temperature, the hysteresis loop becomes more single-phase-like, yet the magnetization remains fully reversible. The interface is characterized via synchrotron x-ray scattering and electron microscopy elemental mapping. The magnetization behavior is modeled by assuming a graded interface where the material parameters vary continuously. The simulations produce demagnetization curves similar to experimental observations.

Evidence for Ligand-Induced Paramagnetism in CdSe Quantum Dots

We report evidence that paramagnetism in CdSe QDs can be induced via manipulation of the surface chemistry. Using SQUID magnetometry and X-ray absorption spectroscopy, we demonstrate that the paramagnetic behavior of the CdSe QDs can be varied by changing the ligand end-group functionality of the passivating layer. Contrary to previous reports, no evidence for ferromagnetism was observed. The results suggest that the paramagnetism is induced via pi back-bonding between Cd 4d orbtials and ligands with empty pi* orbitals.

Pressure-induced electronic mixing and enhancement of ferromagnetic ordering in EuX (X=Te, Se, S, O) magnetic semiconductors.

The pressure- and anion-dependent electronic structure of EuX (X=Te, Se, S, O) monochalcogenides is probed with element- and orbital-specific x-ray absorption spectroscopy in a diamond anvil cell. An isotropic lattice contraction enhances the ferromagnetic ordering temperature by inducing mixing of Eu 4f and 5d electronic orbitals. Anion substitution (Te-->O) enhances competing exchange pathways through spin-polarized anion p states, counteracting the effect of the concomitant lattice contraction. The results have strong implications for efforts aimed at enhancing FM exchange interactions in thin films through interfacial strain or chemical substitutions.

Nature of Ho magnetism in multiferroic HoMnO3.

Using x-ray resonant magnetic scattering and x-ray magnetic circular dichroism, techniques that are element specific, we have elucidated the role of Ho3+ in multiferroic HoMnO3. In zero field, Ho3+ orders antiferromagnetically with moments aligned along the hexagonal c direction below 40 K, and undergoes a transition to another magnetic structure below 4.5 K. In applied electric fields of up to 1 x 10(7) V/m, the magnetic structure of Ho3+ remains unchanged.

Imaging spiral magnetic domains in Ho metal using circularly polarized Bragg diffraction

We have used circularly polarized x rays to image the spiral magnetic domain structure in a single crystal of Ho metal. In these structures, the magnetization direction rotates between successive atomic layers forming a helix. At magnetic Bragg diffraction peaks, circularly polarized x rays are sensitive to the handedness of such a helix (i.e., either right or left handed). By reversing the helicity of the incident beam with phase-retarding optics and measuring the difference in the Bragg scattering, contrast between domains of opposing handedness can be obtained.

A Transition from Localized to Strongly Correlated Electron Behavior and Mixed Valence Driven by Physical or Chemical Pressure in ACo2As2 (A = Eu and Ca)

We demonstrate that the action of physical pressure, chemical compression, or aliovalent substitution in ACo2As2 (A = Eu and Ca) has a general consequence of causing these antiferromagnetic materials to become ferromagnets. In all cases, the mixed valence triggered at the electropositive A site results in the increase of the Co 3d density of states at the Fermi level. Remarkably, the dramatic alteration of magnetic behavior results from the very minor (<0.15 electron) change in the population of the 3d orbitals. The mixed valence state of Eu observed in the high-pressure (HP) form of EuCo2As2 exhibits a remarkable stability, achieving the average oxidation state of +2.25 at 12.6 GPa. In the case of CaCo2As2, substituting even 10% of Eu or La into the Ca site causes ferromagnetic ordering of Co moments. Similar to HP-EuCo2As2, the itinerant 3d ferromagnetism emerges from electronic doping into the Co layer because of chemical compression of Eu sites in Ca0.9Eu0.1Co1.91As2 or direct electron doping in Ca0.85La0.15Co1.89As2. The results reported herein demonstrate the general possibility of amplifying minor localized electronic effects to achieve major changes in materials properties via involvement of strongly correlated electrons.

Reentrant valence transition in EuO at high pressures: beyond the bond-valence model.

The pressure-dependent relation between Eu valence and lattice structure in model compound EuO is studied with synchrotron-based x-ray spectroscopic and diffraction techniques. Contrary to expectation, a 7% volume collapse at ≈45  GPa is accompanied by a reentrant Eu valence transition into a lower valence state. In addition to highlighting the need for probing both structure and electronic states directly when valence information is sought in mixed-valent systems, the results also show that widely used bond-valence methods fail to quantitatively describe the complex electronic valence behavior of EuO under pressure.

Emerging magnetism and anomalous Hall effect in iridate–manganite heterostructures

Strong Coulomb repulsion and spin–orbit coupling are known to give rise to exotic physical phenomena in transition metal oxides. Initial attempts to investigate systems, where both of these fundamental interactions are comparably strong, such as 3d and 5d complex oxide superlattices, have revealed properties that only slightly differ from the bulk ones of the constituent materials. Here we observe that the interfacial coupling between the 3d antiferromagnetic insulator SrMnO3 and the 5d paramagnetic metal SrIrO3 is enormously strong, yielding an anomalous Hall response as the result of charge transfer driven interfacial ferromagnetism. These findings show that low dimensional spin–orbit entangled 3d–5d interfaces provide an avenue to uncover technologically relevant physical phenomena unattainable in bulk materials.