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The topological Hall effect (THE), a quantum phenomenon arising from the emergent magnetic field generated by a topological spin texture, is a key method for detecting non-coplanar spin structures like skyrmions in magnetic materials. Here, we investigate a bilayer structure of Pt and the conducting ferrimagnet NiCo2O4 (NCO) of perpendicular magnetic anisotropy and demonstrate a giant THE across a temperature range of 2–350 K. The absence of THE in a single-layer Pt and NCO, as well as in Pt/Cu/NCO, suggests its interfacial origin. The maximum THE occurring just before the NCO coercive field indicates its connection to magnetic nucleation centers, which are topologically equivalent to skyrmions. The large normalized THE, based on the emergent-field model, points to a high population density of small magnetic nucleation centers. This aligns with the seemingly unresolvable domain structures by the employed techniques during magnetization reversal, even though clear domain structures are detected after zero-field cooling. These results establish heavy metal/NCO as a promising system for exploring topological spin structures. 

Abstract We report on the temperature dependent low energy electron diffraction (LEED) studies of 12 nm epitaxial Sr₃Ir₂O₇(001) thin films. The Debye temperature has been extracted from the temperature-dependence of LEED intensity at elevated temperatures and different electron kinetic energies. For the most surface sensitive LEED, obtained at the lowest electron kinetic energies, the extracted surface Debye temperature is 270 ± 22 K, which is much lower than the 488 ± 40 K Debye temperature obtained using higher electron kinetic energies. Surprisingly, the LEED diffraction intensity, at the lowest electron kinetic energies, increases rather than decreases, with increasing sample temperatures up to about 440 K. This anomalous behavior has been attributed to the reduction of the lattice vibrational amplitudes along the surface normal. This damping of the normal mode vibrations with increasing temperature results from the enhanced electronic screening via thermally activated carriers. This scenario is corroborated by the transport measurement, showing that Sr₃Ir₂O₇is a narrow band Mott insulator with a band gap of about 32 meV. We have identified criteria for finding anomalous scattering behavior in other transition metal oxide systems. 

Abstract From a comparison of the known molecular stoichiometry and x-ray photoemission spectroscopy, it is evident that the Fe(III) spin crossover salt [Fe(qsal)₂Ni(dmit)₂] has a preferential surface termination with the Ni(dmit)₂moiety, where qsal = N(8quinolyl)salicylaldimine, and dmit²⁻= 1,3-dithiol-2-thione-4,5-dithiolato. This preferential surface termination leads to a significant surface to bulk core level shift for the Ni 2p x-ray photoemission core level, not seen in the corresponding Fe 2p core level spectra. A similar surface to bulk core level shift is seen in Pd 3d in the related [Fe(qsal)₂]₂Pd(dmit)₂. Inverse photoemission spectroscopy, compared with the x-ray absorption spectra at the Ni-L3,2 edge provides some indication of the density of states resulting from the dmit²⁻= 1,3-dithiol-2-thione-4,5-dithiolato ligand unoccupied molecular orbitals and thus supports the evidence regarding surface termination in the Ni(dmit)₂moiety. 

Abstract X-ray photoelectron spectroscopy (XPS) shows that dramatic changes in the core level binding energies can provide strong indications of transitions between more dielectric and more metallic CoFe₂O₄and NiCo₂O₄thin films. These significant variations in the XPS core level binding energies are possible with a combination of annealing and oxygen exposure; however, the behaviors of the CoFe₂O₄and NiCo₂O₄thin films are very different. The XPS Co and Fe 2p_3/2core levels for the CoFe₂O₄thin film at room temperature show large photovoltaic surface charging, leading to binding energy shifts, characteristic of a highly dielectric (or insulating) surface at room temperature. The photovoltaic charging, observed in the XPS binding energies of the Co and Fe 2p_3/2core levels, decreases with increasing temperature. The XPS core level binding energies of CoFe₂O₄thin film saturated at lower apparent binding energies above 455 K. This result shows that the prepared CoFe₂O₄thin film can be dielectric at room temperature but become more metallic at elevated temperatures. The dielectric nature of the CoFe₂O₄thin film was restored only when the film was annealed in sufficient oxygen, indicating that oxygen vacancies play an important role in the transition of the film from dielectric (or insulating) to metallic. In contrast, the XPS studies of initially metallic NiCo₂O₄thin film demonstrated that annealing NiCo₂O₄thin film led to a more dielectric or insulating film. The original more metallic character of the NiCo₂O₄film was restored when the NiCo₂O₄was annealed in sufficient oxygen. Effective activation energies are estimated for the carriers from a modified Arrhenius-type model applied to the core level binding energy changes of the CoFe₂O₄and NiCo₂O₄thin films, as a function of temperature. The origin of the carriers, however, is not uniquely identified. This work illustrates routes to regulate the surface metal-to-insulator transition of dielectric oxides, especially in the case of insulating NiCo₂O₄thin film that can undergo reversible metal-to-insulator transition with temperature. 

The spin crossover complex Fe(phen)2(NCS)2 and its composite, Fe(phen)2(NCS)2, combined with the conducting polymer polyaniline (PANI) plus varying concentrations of iron magnetite (Fe3O4) nanoparticles were studied. A cooperative effect is evident from the hysteresis width in the plot of magnetic susceptibility multiplied by temperature versus temperature (χmT versus T) for Fe(phen)2(NCS)2 with PANI plus varying concentrations of Fe3O4 nanoparticles. The hysteresis width in the composites vary no more than 2 K with respect to the pristine Fe(phen)2(NCS)2 spin crossover crystallites despite the fact that there exists a high degree of miscibility of the Fe(phen)2(NCS)2 spin crossover complex with the PANI. The Fe3O4 nanoparticles in the Fe(phen)2(NCS)2 plus PANI composite tend to agglomerate at higher concentrations regardless of the spin state of Fe(phen)2(NCS)2. Of note is that the Fe3O4 nanoparticles are shown to be antiferromagnetically coupled with the Fe(phen)2(NCS)2 when Fe(phen)2(NCS)2 is in the high spin state. 

Abstract Evidence of chirality was observed at the Fe metal center in Fe(III) spin crossover coordination salts [Fe(qsal)₂][Ni(dmit)₂] and [Fe(qsal)₂](TCNQ)₂from x-ray absorption (XAS) spectroscopy at the Fe 2p_3/2core threshold. Based on the circularly polarized XAS data, the x-ray natural circular dichroism for [Fe(qsal)₂][Ni(dmit)₂] and [Fe(qsal)₂](TCNQ)₂is far stronger than seen for [Fe(qsal)₂]Cl suggesting this natural circular dichroism signature is a ligand effect rather than a result of just a loss of octahedral symmetry on the Fe core. The larger the chiral effects in the Fe 2p core to bound XAS, the greater the perturbation of the Fe 2p_3/2to 2p_1/2spin–orbit splitting seen in the XAS spectra. 

Abstract In an effort to reconcile the various interpretations for the cation components of the 2p_3/2observed in x-ray photoelectron spectroscopy (XPS) of several spinel oxide materials, the XPS spectra of both spinel alloy nanoparticles and crystalline thin films are compared. We observed that different components of the 2p_3/2core level XPS spectra, of these inverse spinel thin films, are distinctly surface and bulk weighted, indicating surface-to-bulk core level shifts in the binding energies. Surface-to-bulk core level shifts in binding energies of Ni and Fe 2p_3/2core levels of NiFe₂O₄thin film are observed in angle-resolved XPS. The ratio between surface-weighted components and bulk-weighted components of the Ni and Fe core levels shows appreciable dependency on photoemission angle, with respect to surface normal. XPS showed that the ferrite nanoparticles Ni_xCo_1−xFe₂O₄(x= 0.2, 0.5, 0.8, 1) resemble the surface of the NiFe₂O₄thin film. Surface-to-bulk core level shifts are also observed in CoFe₂O₄and NiCo₂O₄thin films but not as significantly as in NiFe₂O₄thin film. Estimates of surface stoichiometry of some spinel oxide nanoparticles and thin films suggested that the apportionment between cationic species present could be farther from expectations for thin films as compared to what is seen with nanoparticles. 

NiCo2O4 (NCO) films grown on MgAl2O4 (001) substrates have been studied using magnetometry and x-ray magnetic circular dichroism based on x-ray absorption spectroscopy and spin-polarized inverse photoemission spectroscopy with various thicknesses down to 1.6 nm. The magnetic behavior can be understood in terms of a layer of optimal NCO and an interfacial layer (1.2 ± 0.1 nm), with a small canting of magnetization at the surface. The thickness dependence of the optimal layer can be described by the finite-scaling theory with a critical exponent consistent with the high perpendicular magnetic anisotropy. The interfacial layer couples antiferromagnetically to the optimal layer, generating exchange-spring styled magnetic hysteresis in the thinnest films. The non-optimal and measurement-speed-dependent magnetic properties of the interfacial layer suggest substantial interfacial diffusion. 

Abstract Understanding intrinsic exchange bias in nominally single‐component ferromagnetic or ferrimagnetic materials is crucial for simplifying related device architectures. However, the mechanisms behind this phenomenon and its tunability remain elusive, which hinders the efforts to achieve unidirectional magnetization for widespread applications. Inspired by the high tunability of ferrimagnetic inverse spinel NiCo₂O₄, the origin of intrinsic exchange bias in NiCo₂O₄(111) films deposited on Al₂O₃(0001) substrates are investigated. The comprehensive characterizations, including electron diffraction, X‐ray reflectometry and spectroscopy, and polarized neutron reflectometry, reveal that intrinsic exchange bias in NiCo₂O₄(111)/Al₂O₃(0001) arises from a reconstructed antiferromagnetic rock‐salt Ni_xCo_1‐xO layer at the interface between the film and the substrate due to a significant structural mismatch. Remarkably, by engineering the interfacial structure under optimal growth conditions, it can achieve exchange bias larger than coercivity, leading to unidirectional magnetization. Such giant intrinsic exchange bias can be utilized for realistic device applications. This work establishes a new material platform based on NiCo₂O₄, an emergent spintronics material, to study tunable interfacial magnetic and spintronic properties.