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Showing papers on "Curie temperature published in 2007"


Journal ArticleDOI
TL;DR: The proximity to a ferromagnetic instability, the defect sensitivity of T(s), and the absence of Pauli limiting, suggest triplet superconductivity mediated by criticalferromagnetic fluctuations.
Abstract: We report the coexistence of ferromagnetic order and superconductivity in UCoGe at ambient pressure. Magnetization measurements show that UCoGe is a weak ferromagnet with a Curie temperature T(C)=3 K and a small ordered moment m(0)=0.03 micro(B). Superconductivity is observed with a resistive transition temperature T(s)=0.8 K for the best sample. Thermal-expansion and specific-heat measurements provide solid evidence for bulk magnetism and superconductivity. The proximity to a ferromagnetic instability, the defect sensitivity of T(s), and the absence of Pauli limiting, suggest triplet superconductivity mediated by critical ferromagnetic fluctuations.

449 citations


Journal ArticleDOI
TL;DR: In this article, the electronic, magnetic, and structural properties of the binary compound Mn3Ga were investigated and it was found that the material is hard magnetic with an energy product of Hc×Br=52.5kJm−3 and an average saturation magnetization of about 0.25μB∕at at 5K.
Abstract: This work reports about the electronic, magnetic, and structural properties of the binary compound Mn3Ga. The tetragonal DO22 phase of Mn3Ga was successfully synthesized and investigated. It has been found that the material is hard magnetic with an energy product of Hc×Br=52.5kJm−3 and an average saturation magnetization of about 0.25μB∕at. at 5K. The saturation magnetization indicates a ferrimagnetic order with partially compensating moments at the Mn atoms on crystallographically different sites. The Curie temperature is above 730K where the onset of decomposition is observed. The electronic structure calculations indicate a nearly half-metallic ferrimagnetic order with 88% spin polarization at the Fermi energy.

338 citations


Journal ArticleDOI
TL;DR: In this article, a morphotropic phase boundary between orthorhombic and tetragonal ferroelectric phases was identified in the composition range of 0.02
Abstract: Highly dense (1−x)(Na0.5K0.5)NbO3–x(Bi0.5Na0.5)TiO3 (NKN-BST) solid solution piezoelectric ceramics have been fabricated by ordinary sintering. All compositions show pure perovskite structures, showing room-temperature symmetries of orthorhombic at x⩽0.02, of tetragonal at 0.03⩽x⩽0.09, of cubic at 0.09 0.20. A morphotropic phase boundary (MPB) between orthorhombic and tetragonal ferroelectric phases was identified in the composition range of 0.02

316 citations


Journal ArticleDOI
TL;DR: In this paper, the results of X-ray diffraction (XRD), low field AC magnetic susceptibility, DC electrical resistivity and dielectric constant measurements were discussed in terms of polaron hopping model.

311 citations


Journal ArticleDOI
TL;DR: In this article, the electronic structure and magnetism of hypothetical MC (Mg, Ca, Sr, and Ba) compounds with the zinc-blende (ZB) crystal structure were investigated using the first-principles linearized augmented plane-wave method based on density functional theory.
Abstract: Using the first-principles full-potential linearized augmented plane-wave method based on density functional theory, we have investigated the electronic structure and magnetism of hypothetical MC (M=Mg, Ca, Sr, and Ba) compounds with the zinc-blende (ZB) crystal structure. It is shown that ZB CaC, SrC, and BaC are half-metallic ferromagnets with large half-metallic gaps (up to 0.83 eV). The half metallicity is found to be robust with respect to the lattice compression and is maintained up to the lattice-constant contraction of 14%, 13%, and 9% for CaC, SrC, and BaC, respectively. The exchange interactions in these compounds are studied using the augmented spherical wave method in conjunction with the frozen-magnon approach. The Curie temperature is estimated within both the mean field approximation and the random phase approximation. The predicted Curie temperatures of all three half-metallic compounds considerably exceed the room temperature. The large half-metallic gaps, the robustness of the half metallicity with respect to the lattice contraction, and the high Curie temperatures make these systems interesting candidates for applications in spintronic devices. The absence of the transition-metal atoms makes these compounds important model systems for the study of the origin and properties of the half-metallic ferromagnetism of s-p electron systems.

284 citations


Journal ArticleDOI
TL;DR: In this paper, the Curie temperatures for the Heusler compounds Co{sub 2}TiAl, Co-sub 2]VGa, CoSub 2}VSn, Cosub 2 VSn, CrGa, CrAl, MnSi, CoCoSn, and CoCoSi are determined from the electronic structure obtained with the local density functional approximation and/or the generalized gradient approximation.
Abstract: The Curie temperatures for the Heusler compounds Co{sub 2}TiAl, Co{sub 2}VGa, Co{sub 2}VSn, Co{sub 2}CrGa, Co{sub 2}CrAl, Co{sub 2}MnAl, Co{sub 2}MnSn, Co{sub 2}MnSi, and Co{sub 2}FeSi are determined ab initio from the electronic structure obtained with the local-density functional approximation and/or the generalized gradient approximation. Frozen spin spirals are used to model the excited states needed to evaluate the spherical approximation for the Curie temperature. The spherical approximation is found to describe the experimental Curie temperatures very well which, for the compounds selected, extend over the range from 95 to 1100 K; as a function of the valence electron count, they show an approximately linear trend which finds an explanation by our calculations.

282 citations


Journal ArticleDOI
TL;DR: In this article, a tower-shaped entropy change of the height of ∼27J∕kgK is obtained based on the analyses of heat capacity, while the Maxwell relation predicts an extra entropy peak of the length of the tower, slightly varying with the Pr content.
Abstract: Entropy changes in the compounds of La1−xPrxFe11.5Si1.5 (x=0.3 and 0.4) have been experimentally studied. A tower-shaped entropy change of the height of ∼27J∕kgK is obtained based on the analyses of heat capacity, while the Maxwell relation predicts an extra entropy peak of the height of ∼99J∕kgK, slightly varying with Pr content. A careful study indicates that the Maxwell relation cannot be used in the vicinity of the Curie temperature because of the coexistence of paramagnetic and ferromagnetic phases, and the huge entropy peak is a spurious result. Similar conclusions are applicable to MnAs and Mn1−xFexAs, for which huge entropy changes have been reported. Appropriate methods for the determination of entropy change of the compound with phase separation are discussed based on the magnetic data.

229 citations


Journal ArticleDOI
TL;DR: The results imply that nanostructured films with a high density of edge spins can give rise to magnetism even though the bulk material is nonmagnetic.
Abstract: Bulk molybdenum disulfide is known to be a nonmagnetic material. We have synthesized edge-oriented MoS2 nanosheet-like films that exhibit weak magnetism (∼1−2 emu/g) and 2.5% magnetoresistance effects with a Curie temperature of 685 K. The magnetization is related to the presence of edge spins on the prismatic edges of the nanosheets. Spin-polarized calculations were performed on triangular-shaped cluster models in order to provide insight into the origin of magnetism on the edges as well as the size-property correlation in these MoS2 nanosheets. Our results imply that nanostructured films with a high density of edge spins can give rise to magnetism even though the bulk material is nonmagnetic.

228 citations


Journal ArticleDOI
TL;DR: In this paper, a unified physical picture of magnetism and an accurate calculation method of Curie temperature (T C ) in dilute magnetic semiconductors (DMSs) in II-VI and III-V compound compounds was proposed.
Abstract: Based upon ab initio electronic structure calculations by the Korringa-Kohn-Rostoker coherent-potential approximation (KKR-CPA) method within the local-density approximation (LDA), we propose a unified physical picture of magnetism and an accurate calculation method of Curie temperature (T C ) in dilute magnetic semiconductors (DMSs) in II-VI and III-V compound semiconductors. We also propose the unified physical picture of magnetism in the DMS, where ferromagnetic Zener's double-exchange mechanism (or Zener's p-d exchange mechanism) caused by the partially occupied impurity band and anti-ferromagnetic super-exchange mechanism (or ferromagnetic super-exchange mechanism) is competing to determine the magnetic states in the DMS. We propose that the three-dimensional 3D Dairisekiphase and one-dimensional 1D Konbu-phase caused by spinodal nano-decomposition are responsible for high-T C phase in the inhomogeneous system. We propose the new methodology to go beyond LDA to describe the highly correlated electron system by taking into account the self-interaction correction (SIC) to the LDA.

204 citations


Journal ArticleDOI
TL;DR: In this paper, the magnetocaloric properties of polycrystalline Ni50Mn50−xInx (15⩽x ⩽16) were studied using magnetization measurements.
Abstract: The magnetocaloric properties of polycrystalline Ni50Mn50−xInx (15⩽x⩽16) associated with the second order magnetic transition at the Curie temperature and the first order martensitic transition were studied using magnetization measurements. The refrigeration capacity and magnetic entropy change were found to depend on the In concentration and reach a maximum value of refrigeration capacity of 280J∕kg with a magnetic entropy change of −6.8J∕kgK at 318K for a magnetic field change of 5T. These values of the magnetocaloric parameters are comparable to that of the largest values reported near the second order transition of metallic magnets near room temperature.

203 citations


Journal ArticleDOI
TL;DR: In this paper, an osmium-based double perovskite with a Curie temperature of 725 K has been synthesized for spintronic materials with high spin polarization at room temperature.
Abstract: In the search for new spintronic materials with high spin polarization at room temperature, we have synthesized an osmium-based double perovskite with a Curie temperature of 725 K. Our combined exp ...

Journal ArticleDOI
TL;DR: In this paper, structural, electrical, and magnetic properties of Ni1−xZnxFe2O4 (x=0.2, 0.4) samples sintered at various temperatures have been investigated thoroughly.

Journal ArticleDOI
TL;DR: Li Sb O 3 and Sb 5 + diffuse into the lattices to form a perovskite structure as mentioned in this paper, leading to a significant enhancement of the piezoelectric properties.
Abstract: Lead-free piezoelectricceramics ( 1 − x ) K 05 Na 05 Nb O 3 – x Li Sb O 3 have been fabricated by a conventional ceramicsintering technique The results of x-ray diffraction suggest that Li + and Sb 5 + diffuse into the K 05 Na 05 Nb O 3 lattices to form a solid solution with a perovskite structure The ceramics can be well sintered at 1070 – 1110 ° C The introduction of Li Sb O 3 into the Na 05 K 05 Nb O 3 solid solution decreases slightly the paraelectric cubic-ferroelectric tetragonal phase transition temperature ( T c ) , but greatly shifts the ferroelectric tetragonal-ferroelectric orthorhombic phase transition ( T O – F ) to room temperature Coexistence of the orthorhombic and tetragonal phases is formed at 005 < x < 007 at room temperature, leading to a significant enhancement of the piezoelectric properties For the ceramic with x = 006 , the piezoelectric properties become optimum: piezoelectric constant d 33 = 212 pC ∕ N , planar and thickness electromechanical coupling factors k P = 46 % and k t = 47 % , respectively, remanent polarization P r = 150 μ C ∕ cm 2 , coercive field E c = 174 kV ∕ mm , and Curie temperature T C = 358 ° C

Journal ArticleDOI
TL;DR: In this article, the magnetodielectric properties of well-ordered epitaxial La2CoMnO6 films were investigated under applied magnetic fields up to 50kOe.
Abstract: We report on the magnetodielectric properties of well-ordered epitaxial La2CoMnO6 films. The temperature dependence of the dielectric constant is measured in the 10–105Hz frequency range under applied magnetic fields up to 50kOe. As temperature is lowered, the dielectric constant decreases in the ferromagnetic regime and approaches a plateau below 100K. A significant enhancement in the dielectric constant under applied magnetic field is observed only in the ferromagnetic phase regime culminating around the transition temperature, while it is absent in the paramagnetic phase regime. Using Arrott plots, we also demonstrate that these films exhibit a second-order phase transition at their Curie temperature. The observed magnetodielectric characteristics of the films are interpreted using the phenomenological theory.

Journal ArticleDOI
TL;DR: In this paper, measurements of the adiabatic temperature change in the inverse magnetocaloric alloy of the Curie point have been carried out and it is shown that this alloy heats up with the application of a magnetic field around the curie point.
Abstract: We report on measurements of the adiabatic temperature change in the inverse magnetocaloric ${\mathrm{Ni}}_{50}{\mathrm{Mn}}_{34}{\mathrm{In}}_{16}$ alloy. It is shown that this alloy heats up with the application of a magnetic field around the Curie point due to the conventional magnetocaloric effect. In contrast, the inverse magnetocaloric effect associated with the martensitic transition results in the unusual decrease of temperature by adiabatic magnetization. We also provide magnetization and specific heat data which enable to compare the measured temperature changes to the values indirectly computed from thermodynamic relationships. Good agreement is obtained for the conventional effect at the second-order paramagnetic-ferromagnetic phase transition. However, at the first-order structural transition the measured values at high fields are lower than the computed ones. Irreversible thermodynamics arguments are given to show that such a discrepancy is due to the irreversibility of the first-order martensitic transition.

Journal ArticleDOI
TL;DR: In this article, a theoretical study of the magnetism induced in transition metal dioxides ZrO2 and TiO2 by substitution of the cation by a vacancy or an impurity from the groups 1A or 2A of the periodic table, where the impurity is either K or Ca.
Abstract: We perform a theoretical study of the magnetism induced in transition metal dioxides ZrO2 and TiO2 by substitution of the cation by a vacancy or an impurity from the groups 1A or 2A of the periodic table, where the impurity is either K or Ca. In the present study both supercell and embedded cluster methods are used. It is demonstrated that the vacancy and the K-impurity leads to a robust induced magnetic moment on the surrounding O-atoms for both the cubic ZrO2 and rutile TiO2 host crystals. On the other hand it is shown that Ca-impurity leads to a non magnetic state. The native O-vacancy does not induce a magnetic moment in the host dioxide crystal.

Journal ArticleDOI
TL;DR: An experimental formula for producing a set of ceramics with high piezoelectric properties is obtained while cutting down the Ta content and maintaining a high Curie temperature in this paper.
Abstract: Lead-free alkaline niobate based (Na0.52K0.48−xLix)Nb1−x−ySbxTayO3 piezoceramics have been prepared by the conventional mixed oxide method without using other techniques. An experimental formula for producing a set of ceramics with high piezoelectric properties is obtained while cutting down the Ta content and maintaining a high Curie temperature. The highest piezoelectric constant d33 is 308pC∕N, with a dielectric loss tanδ of about 2.0% and a Curie temperature of 339°C. The samples also possess outstanding high-field piezoelectric strain effects. The high-field piezoelectric strain coefficient d33* is as high as 490pm∕V. (Li, Sb, Ta) modified (Na,K)NbO3 shifts the orthorhombic to tetragonal phase transition to near room temperature, which plays an important role in the improvement of the piezoelectric properties.

Journal ArticleDOI
18 Jan 2007-Nature
TL;DR: Magnetic characterization of the three compounds reveals spontaneous field-dependent magnetization and hysteresis at room temperature, with ordering temperatures well above ambient, highlighting these three compounds as members of a class of stable magnets that are at the interface between conventional inorganic magnets and genuine molecule-based magnets.
Abstract: For over two decades there have been intense efforts aimed at the development of alternatives to conventional magnets, particularly materials comprised in part or wholly of molecular components. Such alternatives offer the prospect of realizing magnets fabricated through controlled, low-temperature, solution-based chemistry, as opposed to high-temperature metallurgical routes, and also the possibility of tuning magnetic properties through synthesis. However, examples of magnetically ordered molecular materials at or near room temperature are extremely rare, and the properties of these materials are often capricious and difficult to reproduce. Here we present a versatile solution-based route to a new class of metal-organic materials exhibiting magnetic order well above room temperature. Reactions of the metal (M) precursor complex bis(1,5-cyclooctadiene)nickel with three different organics A-TCNE (tetracyanoethylene), TCNQ (7,7,8,8-tetracyanoquinodimethane) or DDQ (2,3-dichloro-5,6-dicyano-1,4-benzoquinone)--proceed via electron transfer from nickel to A and lead to materials containing Ni(II) ions and reduced forms of A in a 2:1 Ni:A ratio--that is, opposite to that of conventional (low Curie temperature) MA(2)-type magnets. These materials also contain oxygen-based species within their architectures. Magnetic characterization of the three compounds reveals spontaneous field-dependent magnetization and hysteresis at room temperature, with ordering temperatures well above ambient. The unusual stoichiometry and striking magnetic properties highlight these three compounds as members of a class of stable magnets that are at the interface between conventional inorganic magnets and genuine molecule-based magnets.

Journal ArticleDOI
TL;DR: In this paper, relaxor-based ferroelectric single crystals Pb(In1∕2Nb1 ∕2)O3-Pb(Mg 1∕3Nb2 ∕3)-PbTiO3 (PIMNT) have been grown directly from their melt using the vertical Bridgman method, and their boules have reached the size of ϕ45×80mm.
Abstract: Relaxor-based ferroelectric single crystals Pb(In1∕2Nb1∕2)O3–Pb(Mg1∕3Nb2∕3)O3–PbTiO3 (PIMNT) have been grown directly from their melt using the vertical Bridgman method, and their boules have reached the size of ϕ45×80mm. The as-grown PIMNT28/40/32 crystals on the (001) cuts exhibit a dielectric constant e∼5200, dielectric loss tanδ∼0.50%, piezoelectric strain constant d33∼1700–2200pC∕N, electromechanical coupling factors kt∼0.61 and k33∼0.92, coercive field Ec∼10.88kV∕cm, remanent polarization Pr∼46μC∕cm2, Curie temperature TC∼192°C, and rhombohedral to tetragonal phase transition temperature Trt∼119°C. Moreover, their piezoelectric properties show good thermal stability under the heat treatment at 105°C.

Journal ArticleDOI
TL;DR: In this article, the effects of Ag content on the phase structure and piezoelectric properties of O3 lead-free ceramics were mainly studied, and it was shown that the phase structures undergo a transition from orthorhombic to tetragonal phase with increasing x from 0.00 to 0.06.
Abstract: (K0.44−xNa0.52Li0.04Agx)(Nb0.91Ta0.05Sb0.04)O3 lead-free piezoelectric ceramics were prepared by normal sintering. The effects of Ag content on the phase structure and piezoelectric properties of the ceramics were mainly studied. These results show that the phase structure undergoes a transition from orthorhombic to tetragonal phase with increasing x from 0.00 to 0.06. The optimum Ag content enhances the piezoelectric properties, and the Curie temperature increases with increasing x. The ceramics with x=0.02 exhibit enhanced electrical properties (d33∼263pC∕N, kp∼45.3%, TC∼353°C, er∼1478, and tanδ∼2.3%) and good aging characteristics. These results show that the ceramic with x=0.02 is a promising lead-free piezoelectric material.

Journal ArticleDOI
TL;DR: In this paper, a single-phase barium hexaferrite (BaM) was synthesized by co-precipitation and an additional solid state preparative method using high-purity nitrates, oxides and carbonates of iron (111), barium (11) and ammonium hydroxide.


Journal ArticleDOI
TL;DR: In this article, Li+ and Ta5+ diffuse into the K0.5NbO3 lattices to form a solid solution with a perovskite structure, and the substitution of Li+ induces an increase in the Curie temperature and a decrease in the ferroelectric tetragonal-ferroelectric orthorhombic phase transition temperature.
Abstract: Lead-free ceramics (K0.5Na0.5)1−xLix(Nb1−yTay)O3 have been prepared by an ordinary sintering technique. Our results reveal that Li+ and Ta5+ diffuse into the K0.5Na0.5NbO3 lattices to form a solid solution with a perovskite structure. The substitution of Li+ induces an increase in the Curie temperature (TC) and a decrease in the ferroelectric tetragonal–ferroelectric orthorhombic phase transition temperature (TO-T). On the other hand, both TC and TO-T decrease after the substitution of Ta5+. A coexistence of the orthorhombic and tetragonal phases is formed at 0.03

Journal ArticleDOI
TL;DR: In this article, the specific magnetization, the dynamic magnetic susceptibility, and the heat capacity of anion-deficient manganite were investigated, and it was shown that the ferromagnetic matrix of the material under study is characterized by a scatter in the exchange interaction intensities.
Abstract: For La 0.825 3+ Sr 0.175 2 +Mn3+O 2.912 2− anion-deficient manganite, the specific magnetization, the dynamic magnetic susceptibility, and the heat capacity are investigated. This material is found to be an inhomogeneous ferromagnet below the Curie point T C ≈ 122 K, which is much lower than the Curie point determined for the stoichiometric composition (T C ≈ 268 K). An increase in magnetic field by two orders of magnitude leads to an increase in the Curie temperature by ΔT ≈ 12 K. The presence of oxygen vacancies leads to the frustration of a part, namely, V fr ≈ 22%, of the indirect Mn3+-O-Mn3+ exchange interactions, but the spin glass state is not realized. The ferromagnetic matrix of the material under study is characterized by a scatter in the exchange interaction intensities. The heat capacity is found to exhibit an anomalous behavior. Based on the Banerjee magnetic criterion, it is established that the ferromagnet-paramagnet transition observed for La 0.825 3+ Sr 0.175 2+ Mn3+O 2.912 2− anion-deficient manganite is a second-order thermodynamic phase transition. The mechanism and origin of the critical behavior of the system under investigation are discussed.

Journal ArticleDOI
TL;DR: The XPS data collected from Zn(1-x)Co(x)O samples showed a gradual increase in the oxygen concentration, changing the oxygen-deficient undoped ZnO to an excess oxygen state for x = 0.12, indicating that such high Co concentrations and appropriate oxygen stoichiometry may be needed to achieve adequate ferromagnetic exchange coupling between the incorporated Co(2+) ions.
Abstract: We report the results of a detailed investigation of sol?gel-synthesized nanoscale Zn1?xCoxO powders processed at 350??C with 0?x?0.12 to understand how the structural, morphological, optical and magnetic properties of ZnO are modified by Co doping, in addition to searching for the theoretically predicted ferromagnetism. With x increasing to 0.03, both lattice parameters a and c of the hexagonal ZnO decreased, suggesting substitutional doping of Co at the tetrahedral Zn2+ sites. For x>0.03, these trends reversed and the lattice showed a gradual expansion as x approached 0.12, probably due to additional interstitial incorporation of Co. Raman spectroscopy measurements showed a rapid change in the ZnO peak positions for x>0.03, suggesting significant disorder and changes in the ZnO structure, in support of additional interstitial Co doping possibility. Combined x-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance spectroscopy, photoluminescence spectroscopy and diffuse reflectance spectroscopy showed clear evidence for tetrahedrally coordinated high-spin Co2+ ions occupying the lattice sites of ZnO host system, which became saturated for x>0.03. Magnetic measurements showed a paramagnetic behaviour in Zn1?xCoxO with increasing antiferromagnetic interactions as x increased to 0.10. Surprisingly, a weak ferromagnetic behaviour was observed for the sample with x = 0.12 with a characteristic hysteresis loop showing a coercivity Hc~350?Oe, 25% remanence Mr, a low saturation magnetization Ms~0.04?emu?g?1 and with a Curie temperature Tc~540?K. The XPS data collected from Zn1?xCoxO samples showed a gradual increase in the oxygen concentration, changing the oxygen-deficient undoped ZnO to an excess oxygen state for x = 0.12. This indicates that such high Co concentrations and appropriate oxygen stoichiometry may be needed to achieve adequate ferromagnetic exchange coupling between the incorporated Co2+ ions.

Journal ArticleDOI
TL;DR: In this article, the authors have bombarded graphite samples with protons at low temperatures and low fluences to attenuate the large thermal annealing produced during irradiation.
Abstract: We have bombarded graphite samples with protons at low temperatures and low fluences to attenuate the large thermal annealing produced during irradiation. The overall optimization of sample handling allowed us to find Curie temperatures ${T}_{c}\ensuremath{\gtrsim}350\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ at the fluences used. The magnetization versus temperature shows unequivocally a linear dependence, which can be interpreted as due to excitations of spin waves in a two-dimensional Heisenberg model with a weak uniaxial anisotropy.

Journal ArticleDOI
TL;DR: In this article, structural parameters along with magnetic and electrical behavior of nanosize Co-Ni spinel ferrites synthesized by co-precipitation method are reported along with dielectric constants and loss factors as a function of frequency.

Journal ArticleDOI
TL;DR: In this article, the crystal structure of (1−x)NbO3-xCaTiO3 ceramics was investigated, and it was shown that the 0.95NKN-0.05 ceramic is a good candidate material for lead-free piezoelectric materials.
Abstract: The crystal structure of (1−x)(Na0.5K0.5)NbO3-xCaTiO3 ceramics began to change from orthorhombic to tetragonal at x≥0.03, then became a morphotropic phase boundary in which both the orthogonal and tetragonal phases coexisted at 0.03

Journal ArticleDOI
TL;DR: In this paper, it was shown that perovskite cobaltite (La{sub 1?x}Sr{sub x}CoO{sub 3}) exhibits a clustered state above the Curie point in the ferromagnetic phase.
Abstract: The existence of preformed clusters above the Curie temperature of the doped perovskite manganites is well established and, in many cases, conforms to the expectations for a Griffiths phase. We show here that the canonical perovskite cobaltite (La{sub 1?x}Sr{sub x}CoO{sub 3}) also exhibits a clustered state above the Curie point in the ferromagnetic phase. The formation of magnetic clusters at a well-defined temperature (T*) is revealed in the small-angle neutron scattering and dc susceptibility. Remarkably, the characteristics of this clustered state appear quite unlike those of a Griffiths phase; the deviation from Curie-Weiss behavior is opposite to expectations and is field independent, while T* does not correspond to the undiluted Curie temperature. These results demonstrate that, although the Griffiths model may apply to many systems with quenched disorder, it is not universally applicable to randomly doped transition metal oxides.

Journal ArticleDOI
TL;DR: In this paper, the presence of ferromagnetic signatures was linked to the formation of Fe-rich nanocrystals, as evidenced by high-resolution x-ray diffraction, transmission electron microscopy (TEM), spatially resolved energy dispersive xray spectroscopy (EDS), secondary-ion mass spectraopy (SIMS), photoluminescence (PL), electron-paramagnetic resonance (EPR), and magnetometry employing a superconducting quantum interference device (SQUID).
Abstract: We report on the metalorganic chemical vapor deposition of $\mathrm{GaN}:\mathrm{Fe}$ and $(\mathrm{Ga},\mathrm{Fe})\mathrm{N}$ layers on $c$-sapphire substrates and their thorough characterization via high-resolution x-ray diffraction, transmission electron microscopy (TEM), spatially resolved energy dispersive x-ray spectroscopy (EDS), secondary-ion mass spectroscopy (SIMS), photoluminescence (PL), Hall-effect, electron-paramagnetic resonance (EPR), and magnetometry employing a superconducting quantum interference device (SQUID). A combination of TEM and EDS reveals the presence of coherent nanocrystals presumably ${\mathrm{Fe}}_{x}\mathrm{N}$ with the composition and lattice parameter imposed by the host. From both TEM and SIMS studies, it is stated that the density of nanocrystals and, thus the Fe concentration increases towards the surface. According to Hall effect measurements, electrons from residual donors are trapped by midgap Fe acceptor states in the limit of low iron content $x\ensuremath{\lesssim}0.4%$, indicating that the concentration of ${\mathrm{Fe}}^{2+}$ ions increases at the expense of Fe ions in the $3+$ charge state. This effect is witnessed by PL measurements as changes in the intensity of the ${\mathrm{Fe}}^{3+}$-related intraionic transition, which can be controlled by codoping with Si donors and Mg acceptors. In this regime, EPR of ${\mathrm{Fe}}^{3+}$ ions and Curie-like magnetic susceptibility are observed. As a result of the spin-orbit interaction, ${\mathrm{Fe}}^{2+}$ does not produce any EPR response. However, the presence of Fe ions in the $2+$ charge state may account for a temperature-independent Van Vleck--type paramagnetic signal that we observe by SQUID magnetometry. Surprisingly, at higher Fe concentrations, the electron density is found to increase substantially with the Fe content. The coexistence of electrons in the conduction band and Fe in the $3+$ charge state is linked to the gradient in the Fe concentration. In layers with iron content $x\ensuremath{\gtrsim}0.4%$ the presence of ferromagnetic signatures, such as magnetization hysteresis and spontaneous magnetization, have been detected. A set of precautions has been undertaken in order to rule out possible sources of spurious ferromagnetic contributions. Under these conditions, a ferromagneticlike response is shown to arise from the $(\mathrm{Ga},\mathrm{Fe})\mathrm{N}$ epilayers, it increases with the iron concentration, it persists up to room temperature, and it is anisotropic---i.e., the saturation value of the magnetization is higher for in-plane magnetic field. We link the presence of ferromagnetic signatures to the formation of Fe-rich nanocrystals, as evidenced by TEM and EDS studies. This interpretation is supported by magnetization measurements after cooling in and without an external magnetic field, pointing to superparamagnetic properties of the system. It is argued that the high temperature ferromagnetic response due to spinodal decomposition into regions with small and large concentration of the magnetic component is a generic property of diluted magnetic semiconductors and diluted magnetic oxides showing high apparent Curie temperature.