Tailoring Interfacial Exchange Anisotropy in Hard–Soft Core-Shell Ferrite Nanoparticles for Magnetic Hyperthermia Applications

Magnetically hard–soft core-shell ferrite nanoparticles are synthesized using an organometallic decomposition method through seed-mediated growth. Two sets of core-shell nanoparticles (S1 and S2) with different shell (Fe3O4) thicknesses and similar core (CoFe2O4) sizes are obtained by varying the initial quantities of seed nanoparticles of size 6.0 ± 1.0 nm. The nanoparticles synthesized have average sizes of 9.5 ± 1.1 (S1) and 12.2 ± 1.7 (S2) nm with corresponding shell thicknesses of 3.5 and 6.1 nm. Magnetic properties are investigated under field-cooled and zero-field-cooled conditions at several temperatures and field cooling values. Magnetic heating efficiency for magnetic hyperthermia applications is investigated by measuring the specific absorption rate (SAR) in alternating magnetic fields at several field strengths and frequencies. The exchange bias is found to have a nonmonotonic and oscillatory relationship with temperature at all fields. SAR values of both core-shell samples are found to be considerably larger than that of the single-phase bare core particles. The effective anisotropy and SAR values are found to be larger in S2 than those in S1. However, the saturation magnetization displays the opposite behavior. These results are attributed to the occurrence of spin-glass regions at the core-shell interface of different amounts in the two samples. The novel outcome is that the interfacial exchange anisotropy of core-shell nanoparticles can be tailored to produce large effective magnetic anisotropy and thus large SAR values.

Zero-field skyrmionic states and in-field edge-skyrmions induced by boundary tuning

When magnetic skyrmions are moved via currents, they do not strictly travel along the path of the current, instead their motion also gains a transverse component. This so-called skyrmion Hall effect can be detrimental in potential skyrmion devices because it drives skyrmions towards the edge of their hosting material where they face potential annihilation. Here we experimentally modify a skyrmion model system—an atomic Pd/Fe bilayer on Ir(111)—by decorating the film edge with ferromagnetic Co/Fe patches. Employing spin-polarized scanning tunneling microscopy, we demonstrate that this ferromagnetic rim prevents skyrmion annihilation at the film edge and stabilizes skyrmions and target states in zero field. Furthermore, in an external magnetic field the Co/Fe rim can give rise to skyrmions pinned to the film edge. Spin dynamics simulations reveal how a combination of different attractive and repulsive skyrmion-edge interactions can induce such an edge-pinning effect for skyrmions.

Cross-Scale Synthesis of Organic High-k Semiconductors Based on Spiro-Gridized Nanopolymers

High dielectric constants in organic semiconductors have been identified as a central challenge for the improvement in not only piezoelectric, pyroelectric, and ferroelectric effects but also photoelectric conversion efficiency in OPVs, carrier mobility in OFETs, and charge density in charge-trapping memories. Herein, we report an ultralong persistence length (lp≈41 nm) effect of spiro-fused organic nanopolymers on dielectric properties, together with excitonic and charge carrier behaviors. The state-of-the-art nanopolymers, namely, nanopolyspirogrids (NPSGs), are synthesized via the simple cross-scale Friedel-Crafts polygridization of A2B2-type nanomonomers. The high dielectric constant (k=8.43) of NPSG is firstly achieved by locking spiro-polygridization effect that results in the enhancement of dipole polarization. When doping into a polystyrene-based dielectric layer, such a high-k feature of NPSG increases the field-effect carrier mobility from 0.20 to 0.90 cm2 V-1 s-1 in pentacene OFET devices. Meanwhile, amorphous NPSG film exhibits an ultralow energy disorder (<50 meV) for an excellent zero-field hole mobility of 3.94×10−3 cm2 V−1 s−1, surpassing most of the amorphous π-conjugated polymers. Organic nanopolymers with high dielectric constants open a new way to break through the bottleneck of efficiency and multifunctionality in the blueprint of the fourth-generation semiconductors.

Muon spin rotation and relaxation study on topological noncentrosymmetric superconductor PbTaSe2

Topological superconductivity is an exotic phenomenon due to the symmetry-protected topological surface state, in which a quantum system has an energy gap in the bulk but supports gapless excitations conned to its boundary. Symmetries including central and time-reversal, along with their relations with topology, are crucial for topological superconductivity. We report muon spin relaxation/rotation (μSR) experiments on a topological noncentrosymmetric superconductor PbTaSe2 to study its TRS and gap symmetry. Zero-field μSR experiments indicate the absence of internal magnetic eld in the superconducting state, consistent with previous μSR results. Furthermore, transverse-field μSR measurements reveals that the superconducting gap of PbTaSe2 is an isotropic three-dimensional fully-gapped single-band. The fully-gapped results can help understand the pairing mechanism and further classify the topological superconductivity in this system.

Is [ReCl4(CN)2]2− a good Building Block for Single Molecule Magnets? A Theoretical Investigation.

Building blocks containing $5d$ spin centres are promising for constructing single molecule magnets due to their large spin-orbit interaction, but experimental and computational results obtained so far indicate that this might not be the case for Re$^\textrm{IV}$ centres in an octahedral environment. Density functional results obtained in this work for [ReCl$_4$(CN)$_2$]$^{2-}$ and trinuclear complexes formed by attaching Mn$^\textrm{II}$ centres to the cyano ligands indicate that zero field splitting in such complexes exhibits large rhombicity (which leads to fast relaxation of the magnetisation) even if there are only small distortions from an ideal geometry with a four-fold symmetry axis. This is already apparent if second-order spin-orbit perturbation theory is applied but even more pronounced if higher-order spin-orbit effects are included as well, as demonstrated by wavefunction based calculations. Computational results are cast into a ligand field model and these simulations show that especially a distortion which is not along the $C_4/C_2$ axeshas a large effect on the rhombicity. Quantum simulations on these complexes are difficult because the zero field splitting strongly depends on the energetic position of the low-lying doublets from the $t_{2g}^3$ configuration.

Oscillating paramagnetic Meissner effect and Berezinskii–Kosterlitz–Thouless transition in Bi2Sr2CaCu2O8+δ monolayer

Monolayers of a prototypical cuprate high transition-temperature (TC) superconductor Bi2Sr2CaCu2O8+δ (Bi2212) was recently found to show TC and other electronic properties similar to those of the bulk. The robustness of superconductivity in an ideal two-dimensional (2D) system was an intriguing fact that defied the Mermin-Wagner theorem. Here, we took advantage of the high sensitivity of scanning SQUID susceptometry to image the phase stiffness throughout the phase transition of Bi2212 in the 2D limit. We found susceptibility oscillated with flux between diamagnetism and paramagnetism in a Fraunhofer-like pattern up till TC. The temperature and sample size-dependence of the modulation period agreed well with our Coulomb gas analogy of a finite 2D system based on Berezinskii–Kosterlitz–Thouless (BKT) transition. In the multilayers, the susceptibility oscillation differed in a small temperature regime below TC in consistent with a dimensional-crossover led by interlayer coupling. Serving as strong evidence of BKT transition in the bulk, there appeared a sharp superfluid density jump at zero-field and paramagnetism at small fields just below TC. These results unified the phase transitions from the monolayer Bi2212 to the bulk as BKT transition with finite interlayer coupling. This elucidating picture favored the pre-formed pairs scenario for the underdoped cuprates regardless of lattice dimensionality.

Широкополосная ЭПР-спектроскопия кристалла SrY-=SUB=-2-=/SUB=-O-=SUB=-4-=/SUB=-:Ho-=SUP=-3+-=/SUP=-

EPR spectra of impurity Ho3+ ions in oriented SrY2O4 single-crystals are registered at the temperature 4.2 K in the frequency range from 70 to 180 GHz. The results of measurements evidence for the substitution of Ho3+ ions for the Y3+ ions at the structurally nonequivalent sites R1 and R2 with the local Cs point symmetry. The values of g-factors, hyperfine structure constants and the energy gaps berween the ground and the first excited non-degenherate crystal-field sublevels of the ground 5I8 multiplet are determined. The observed specific features of the ground states of Но3+ ions (non-Kramers doublets with the zero-field splittings of 4.30 and 1.67 cm-1) open a possibility to identify transitions in optical spectra of SrY2O4:Ho and inelastic neutron scattering spectra of SrHo2O4 crystals.

FeIII in a high-spin state in bis(5-bromosalicylaldehyde 4-ethylthiosemicarbazonato-κ3 O,N 1,S)ferrate(III) nitrate monohydrate, the first example of such a cationic FeIII complex unit

The synthesis and crystal structure (100 K) of the title compound, [Fe(C10H11BrN3OS)2]NO3·H2O, is reported. The asymmetric unit consists of an octahedral [FeIII(HL)2]+ cation, where HL − is H-5-Br-thsa-Et or 5-bromosalicylaldehyde 4-ethylthiosemicarbazonate(1−) {systematic name: 4-bromo-2-[(4-ethylthiosemicarbazidoidene)methyl]phenolate}, a nitrate anion and a noncoordinated water molecule. Each HL − ligand binds via the thione S, the imine N and the phenolate O atom, resulting in an FeIIIS2N2O2 chromophore. The ligands are orientated in two perpendicular planes, with the O and S atoms in cis and the N atoms in trans positions. This [Fe(HL)2](anion)·H2O compound contains the first known cationic FeIII entity containing two salicylaldehyde thiosemicarbazone derivatives. The FeIII ion is in the high-spin state at 100 K. In addition, a comparative IR spectroscopic study of the free ligand and the ferric complex is presented, demonstrating that such an analysis provides a quick identification of the degree of deprotonation and the coordination mode of the ligand in this class of metal compounds. The variable-temperature magnetic susceptibility measurements (5–320 K) are consistent with the presence of a high-spin FeIII ion with a zero-field splitting D = 0.439 (1) cm−1.

De Novo Calculation of the Charge Carrier Mobility in Amorphous Small Molecule Organic Semiconductors

Organic semiconductors (OSC) are key components in applications such as organic photovoltaics, organic sensors, transistors and organic light emitting diodes (OLED). OSC devices, especially OLEDs, often consist of multiple layers comprising one or more species of organic molecules. The unique properties of each molecular species and their interaction determine charge transport in OSCs—a key factor for device performance. The small charge carrier mobility of OSCs compared to inorganic semiconductors remains a major limitation of OSC device performance. Virtual design can support experimental R&amp;D towards accelerated R&amp;D of OSC compounds with improved charge transport. Here we benchmark a de novo multiscale workflow to compute the charge carrier mobility solely on the basis of the molecular structure: We generate virtual models of OSC thin films with atomistic resolution, compute the electronic structure of molecules in the thin films using a quantum embedding procedure and simulate charge transport with kinetic Monte-Carlo protocol. We show that for 15 common amorphous OSC the computed zero-field and field-dependent mobility are in good agreement with experimental data, proving this approach to be an effective virtual design tool for OSC materials and devices.