In this work we report the synthesis and structural, electronic and magnetic properties of La1.5Ca0.5CoMnO6 double-perovskite. This is a re-entrant spin cluster material which exhibits a non-negligible negative exchange bias effect when it is cooled in zero magnetic field from an unmagnetized state down to low temperature. X-ray powder diffraction, X-ray photoelectron spectroscopy and magnetometry results indicate mixed valence state at Co site, leading to competing magnetic phases and uncompensated spins at the magnetic interfaces. We compare the results for this Ca-doped material with those reported for the resemblant compound La1.5Sr0.5CoMnO6, and discuss the much smaller spontaneous exchange bias effect observed for the former in terms of its structural and magnetic particularities. For La1.5Ca0.5CoMnO6, when successive magnetization loops are carried, the spontaneous exchange bias field inverts its sign from negative to positive from the first to the second measurement. We discuss this behavior based on the disorder at the magnetic interfaces, related to the presence of a glassy phase. This compound also exhibits a large conventional exchange bias, for which there is no sign inversion of the exchange bias field for consecutive cycles.
The dependence of thermally induced spontaneous magnetization reversal on time-dependent cooling protocols was studied. Slower cooling and longer waiting close to the Nèel temperature of the antiferromagnet ($T_N$) enhances the magnetization reversal. Cycling the temperature around $T_N$ leads to a thermal training effect under which the reversal magnitude increases with each cycle. These results suggest that spontaneous magnetization reversal is energetically favored, contrary to our present understanding of positive exchange bias.
The magnetic properties of a nanoscale system are inextricably linked to its local environment. In ad-atoms on surfaces and inorganic layered structures the exchange interactions result from the relative lattice positions, layer thicknesses and other environmental parameters. Here, we report on a sample-dependent sign inversion of the magnetic exchange coupling between the three unpaired spins of an organic triradical molecule embedded in a three-terminal device. This ferro-to-antiferromagnetic transition is due to structural distortions and results in a high-to-low spin ground state change in…
We report a giant zero field cooled exchange bias (ZEB) effect (~0.65 T) in La1.5Sr0.5CoMnO6 sample. Magnetic study has revealed a reentrant spin glass ~90 K, phase separation to spin glass and ferromagnetic phases below 50 K and canted antiferromagnetic transition ~10 K. A small conventional exchange bias (CEB) is established with the advent of spontaneous phase separation down to 10 K. Giant ZEB and enhanced CEB effects are found only below 10 K and are attributed to the large unidirectional anisotropy at the interface of isothermally field induced ferromagnetic phase and canted antiferromag…
Exchange biased composites of ferromagnetic single-domain Ni nanoparticles embedded within large grains of MnO have been prepared by reduction of Ni$_x$Mn$_{1-x}$O$_4$ phases in flowing hydrogen. The Ni precipitates are 15-30 nm in extent, and the majority are completely encased within the MnO matrix. The manner in which the Ni nanoparticles are spontaneously formed imparts a high ferromagnetic- antiferromagnetic interface/volume ratio, which results in substantial exchange bias effects. Exchange bias fields of up to 100 Oe are observed, in cases where the starting Ni content $x$ in the precur…
In this work we propose an alternative model to explain the spontaneous exchange bias (SEB) effect observed in spin glass (SG)-like systems. As in a previously proposed model (Ref. 1), it is based on the unconventional dynamics of the SG-like moments at the magnetic hysteresis cycle. However, using a reliable estimate of the amount of SG-spins that are relaxing during the cycle, the new model can correctly describe the changes in the SEB observed for measurements performed at different temperatures and different maximum applied fields.
The structural, electronic, and magnetic properties of La2-xBaxCoMnO6 (0.25 =< x =< 1.0) compounds were investigated employing x-ray powder diffraction and magnetometry. The crystal structure evolves from orthorhombic Pnma to rhombohedral R-3c and then to hexagonal P63/mmc space group as the Ba concentration increases. The magnetization as a function of temperature measurements revealed a ferromagnetic-like behavior for all samples, but antiferromagnetic interactions seem to also be present throughout the whole series. The competition between magnetic phases leads to the phenomenon of spontane…
Zero field cooled spontaneous exchange bias (SEB) is observed in epitaxial La0.7Sr0.3MnO3 (LSMO):NiO self-assembled nanocomposite thin films grown on (001) SrTiO3 single crystal substrate by pulsed laser deposition. SEB is displayed by the novel asymmetry in the hysteresis loop of the composite film along with the field cooled conventional exchange bias (CEB) effect. The training effect shows that exchange bias relaxation is disorder mediated. It is revealed from DC magnetization results that such nanocomposite film divulges spin glass like behaviour, which is arising due to competing ferromag…
Structural, electronic and magnetic properties of polycrystalline La2-xCaxCoMnO6 (0 $\leq$ x $\leq$ 0.75) compounds are investigated by x-ray diffraction and magnetometry. All the samples have an orthorhombic structure and show a slight decrease in the unit cell with Ca-doping. Temperature-dependent magnetization measurements reveal a complex magnetic behavior with two ferromagnetic transitions. These transitions are ascribed to Co2+--Mn4+ and Co3+--Mn3+ couplings and suggest the presence of additional antiferromagnetic couplings in these disordered compounds. Field-dependent magnetization cur…
We report the magnetic and dielectric behavior of Pb6Ni9(TeO6)5, a new compound comprising the honeycomb-like layers of S=1 spins, through detailed structural, magnetic and dielectric investigation. An antiferromagnetic-type transition at 25 K (TN) with weak-ferromagnetic behavior is revealed. Interestingly, a large value of coercive field of 1.32 T at 2 K is observed. The isothermal magnetization after zero-field-cooled condition, it exhibits the presence of large spontaneous exchange bias (SEB) with a magnitude of 0.19 T at 2 K; which is rare in single bulk materials, especially without exte…
We observe an enormous $\textit{spontaneous}$ exchange bias ($\sim$300-600 Oe) - measured in an unmagnetized state following zero-field cooling - in a nanocomposite of BiFeO$_3$ ($\sim$94%)-Bi$_2$Fe$_4$O$_9$ ($\sim$6%) over a temperature range 5-300 K. Depending on the path followed in tracing the hysteresis loop - positive (p) or negative (n) - as well as the maximum field applied, the exchange bias ($H_E$) varies significantly with $\mid-H_{Ep}\mid$ $>$ $\mid H_{En}\mid$. The temperature dependence of $H_E$ is nonmonotonic. It increases, initially, till $\sim$150 K and then decreases as the …
La$_{1.5}$Ba$_{0.5}$CoMnO$_{6}$ is a re-entrant cluster glass material exhibiting a robust negative exchange bias (EB) effect even after being cooled from an unmagnetized state down to low temperature in zero magnetic field. Here we thoroughly investigate this phenomena by performing magnetization as a function of applied field [$M(H)$] measurements at several different temperatures and maximum applied magnetic fields ($H_m$). The spontaneous EB (SEB) effect is observed below 20 K, and shows a maximum value for $H_m$ = 75 kOe. The effect is greatly enhanced when the $M(H)$ curves are measured …
The spontaneous exchange bias (SEB) effect is a remarkable phenomenon recently observed in some reentrant spin-glass materials. Here we investigate the SEB in La$_{1.5}$(Sr$_{0.5-x}$Ba$_{x}$)CoMnO$_{6}$ double-perovskites, a system with multifarious magnetic phases for which a notable increase in the exchange bias field is observed for intermediate Sr/Ba concentrations. The Ba to Sr substitution leads to the enhancement of the crystal lattice, which is accompanied by the raise of both the effective magnetic moment ($μ_{eff}$) and the antiferromagnetic (AFM) transition temperature that is obser…
Interface effect in complex oxide thin film heterostructures lies at the vanguard of current research to design technologically relevant functionality and explore emergent physical phenomena. While most of the previous works focus on the perovskite/perovskite heterostructures, the study on perovskite/brownmillerite interfaces remain at its infancy. Here, we investigate spontaneously stabilized perovskite-ferromagnet (SrCoO3-δ)/brownmillertite-antiferromagnet (SrCoO2.5) bi-layer with TN > TC and discover an unconventional interfacial magnetic exchange bias effect. From magnetometry investigatio…
Topological spin structures, such as magnetic skyrmions, hold great promises for data storage applications, thanks to their inherent stability. In most cases, skyrmions are stabilized by magnetic fields in non-centrosymmetric systems displaying the chiral Dzyaloshinskii-Moriya exchange interaction, while spontaneous skyrmion lattices have been reported in centrosymmetric itinerant magnets with long-range interactions. Here, a spontaneous anti-biskyrmion lattice with unique topology and chirality is predicted in the monolayer of a semiconducting and centrosymmetric metal halide, NiI$_2$. Our fi…
The mechanism of spontaneous exchange bias (SEB) and the dominant factor of its blocking temperature are still unclear in Heusler alloys. Here, the related investigations are performed in Mn2Ni1.5Al0.5 Heusler alloys with SEB. The results of both magnetic measurements and first-principles calculations confirmed that spin frustrated and unfrustrated antiferromagnetic (AFM) states coexist there and they have different magnetic anisotropies, which are essential for SEB. Based on a series of measurement strategies, we demonstrate that the frustrated AFM state undergoes a first-order magnetic trans…
La$_{1.5}$Sr$_{0.5}$CoMn$_{0.5}$Fe$_{0.5}$O$_{6}$ (LSCMFO) compound was prepared by solid state reaction and its structural, electronic and magnetic properties were investigated. The material forms in rhombohedral $R\bar{3}c$ structure, and the presence of distinct magnetic interactions leads to the formation of a Griffiths phase above its FM transition temperature (150 K), possibly related to the nucleation of small short-ranged ferromagnetic clusters. At low temperatures, a spin glass-like phase emerges and the system exhibits both the conventional and the spontaneous exchange bias (EB) effe…
The non-equilibrium cation site occupancy in nanosized zinc ferrites (6-13 nm) with different degree of inversion (0.2 to 0.4) was investigated using Fe and Zn K-edge x-ray absorption spectroscopy XANES and EXAFS, and magnetic measurements. The very good agreement between experimental and ab-initio calculations on the Zn K-edge XANES region clearly show the large Zn2+(A)--Zn2+[B] transference that takes place in addition to the well-identified Fe3+[B]--Fe3+(A) one, without altering the long-range structural order. XANES spectra features as a function of the spinel inversion were shown to depen…
We report on the consequences of non-uniform exchange in magnetic systems. The quantum mechanical exchange interaction between spins is responsible for the phenomenon of magnetic order, and is generally considered to be uniform across bulk magnetic systems. Partly inspired by the Dzyaloshinskii-Moriya interaction--also known as antisymmetric exchange--we use a linearly varying exchange interaction along a magnetic strip as a route to spatial inversion symmetry-breaking. We find that, in addition to asymmetric modes and localization, spatially-varying exchange can be used to design nonreciproca…
We have observed a large as well as path-dependent spontaneous exchange bias (H$_{SEB}$) ($\sim$30-60 mT) in a nanocomposite of BiFeO$_3$-Bi$_2$Fe$_4$O$_9$ across 5-300 K when it is measured in an unmagnetized state following zero-field cooling and appropriate demagnetization. The path dependency yields a variation in the exchange bias depending on the sign of the starting field and the path followed in tracing the hysteresis loop. The asymmetry thus observed - $Δ$H$_{SEB}$ - is found to be decreasing nonmonotonically across 5-300 K with a peak around 200 K. The $Δ$H$_{SEB}$ together with larg…
We present thermodynamic and neutron scattering measurements on the quantum spin ice candidate Nd$_2$Zr$_2$O$_7$. The parameterization of the anisotropic exchange Hamiltonian is refined based on high-energy-resolution inelastic neutron scattering data together with thermodynamic data using linear spin wave theory and numerical linked cluster expansion. Magnetic phase diagrams are calculated using classical Monte Carlo simulations with fields along \mbox{[100]}, \mbox{[110]} and \mbox{[111]} crystallographic directions which agree qualitatively with the experiment. Large hysteresis and irrevers…
Doping at the rare-earth site by divalent alkaline-earth ions in perovskite lattice has witnessed a variety of magnetic and electronic orders with spatially correlated charge, spin and orbital degrees of freedom. Here, we report an antisite disorder driven spontaneous exchange bias effect as a result of hole carrier (Sr2+) doping in La2-xSrxCoMnO6 (0 < x < 1) double perovskites. X-ray diffraction and Raman spectroscopy have evidenced an increase in disorder with the increase of Sr content up to x = 0.5 and thereby decreases from x = 0.5 to 1. X-ray absorption spectroscopy has revealed that onl…
We report the new results of exchange bias effect in Nd_{1-x}Sr_{x}CoO_3 for x = 0.20 and 0.40, where the exchange bias phenomenon is involved with the ferrimagnetic (FI) state in a spontaneously phase separated system. The zero-field cooled magnetization exhibits the FI (T_{FI}) and ferromagnetic (T_C) transitions at ~ 23 and \sim 70 K, respectively for x = 0.20. The negative horizontal and positive vertical shifts of the magnetic hysteresis loops are observed when the system is cooled through T_{FI} in presence of a positive static magnetic field. Training effect is observed for x = 0.20, wh…
Epitaxial inversion of spontaneous polarization in ε-Ga2O3
Nanjing University of Posts and Telecommunications（南京邮电大学）；The Hong Kong University of Science and Technology (Guangzhou)（香港科技大学（广州））；The Hong Kong University of Science and Technology（香港科技大学）
In this work we carried out systematic experimental and theoretical investigations of the ferromagnetic (FMR) response of quasi-two-dimensional magnetic nano-objects - microscopically long nanostripes made of ferromagentic metals. We were interested in the impact of the symmetries of this geometry on the FMR response. Three possible scenarios, from which the inversion symmetry break originated, were investigated:(1) from the shape of the stripe cross-section, (2) from the double-layer structure of the stripes with exchange coupling between the layers, and (3) from the single-side incidence of …
We show that electric currents are induced in inversion asymmetric ferromagnets if the exchange splitting varies in time after excitation by laser pulses. We interpret this phenomenon as the magnetic variant of the inverse Edelstein effect. Based on \textit{ab initio} calculations we determine the size of this effect in Co/Pt(111) and Mn/W(001) magnetic bilayer systems and investigate its dependence on the magnetization direction. The comparison of our theoretical results to experiments measuring the THz signal emitted after laser excitation suggests that ultrafast demagnetization in 3$d$ tran…
Manipulating spin currents in magnetic insulators is a key technology in spintronics. We theoretically study a simple inversion-asymmetric model of quantum antiferromagnets, where both the exchange interaction and the magnetic field are staggered. We calculate spin currents generated by external electric and magnetic fields by using a quantum master equation. We show that an ac electric field with amplitude $E_0$ leads, through exchange-interaction modulation, to the dc and second-harmonic spin currents proportional to $E_0^2$. We also show that dc and ac staggered magnetic fields $B_0$ genera…
The realization of magnetic skyrmions in nanostructures holds great promise for both fundamental research and device applications. Despite recent progress, intrinsic magnetic skyrmions in two-dimensional lattice are still rarely explored. Here, using first-principles calculations and Monte-Carlo simulations, we report the identification of spontaneous magnetic skyrmions in single-layer CrInX3 (X = Te, Se). Due to the joint effect of broken inversion symmetry and strong spin-orbit coupling, inherent large Dzyaloshinskii-Moriya interaction occurs in both systems, endowing the intriguing Neel-typ…
We report the observation of unusual exchange bias phenomena in the doped perovskite cobaltites La_{1-x}Sr_{x}CoO_{3} (x = 0.15, 0.18, and 0.30) in which a spontaneous phase separation into ferromagnetic clusters embedded in a non-ferromagnetic matrix occurs. When the La_{1-x}Sr_{x}CoO_{3} samples are cooled in a static magnetic field through a freezing temperature, the magnetization hysteresis loops exhibit exchange bias, i.e., the loops shift to the negative field and the magnetization becomes asymmetric. Moreover, exchange bias disappears when the measuring magnetic field is high enough. Th…
Exchange bias (EB) refers to a shift of the hysteresis loop along the field axis in materials consisting of ferromagnetic (FM) and antiferromagnetic (AFM) layers, generally after a cooling procedure in high magnetic field. This effect is highly desirable for technological applications ranging from spintronics to magnetic recording. Achieving giant EB effect near room temperature in a small cooling field is thus an on-going technologically relevant challenge for the materials science community. In this work, we present the experimental realization of such a fundamental goal by demonstrating the…
We developed a Landau type theory for the description of polar phenomena in low-dimensional transition metal dichalcogenides (TMDs), specifically exploring flexoelectric origin of the polarization induced by a spontaneous bending and by inversion symmetry breaking due to the interactions with substrate. We consider the appearance of the spontaneous out-of-plane polarization due to the flexoelectric coupling with the strain gradient of the spontaneous surface rippling and surface-induced piezoelectricity. Performed calculations proved that the out-of-plane spontaneous polarization, originated f…
