Low temperature cluster glass behavior in Nd5Ge3

Various experimental evidence obtained from dc and ac magnetization measurements indicates that Nd(5)Ge(3) undergoes a spin glass transition from a high temperature antiferromagnetic state. Below the Néel temperature of 49 K, it shows distinct properties that characterize a cluster glass state, thereby indicating that it is an example of a reentrant spin glass system. Dynamical behavior of the magnetic susceptibility and the magnetic relaxation clearly give evidence of frustration in the material. Geometric frustration arising from the triangular arrangement of Nd atoms seems to be the main reason behind the spin glass state. A field-induced structural distortion accompanying the Néel transition may also be responsible for the frustration and the spin glass state.     

Cluster glass magnetism in the phase-separated Nd2/3Ca1/3MnO3 perovskite

A detailed study of the low-temperature magnetic state and the relaxation in the phase-separated colossal magnetoresistance Nd_2/3Ca_1/3MnO₃ perovskite has been carried out. Clear experimental evidence of the cluster-glass magnetic behavior of this compound has been revealed. Well defined maxima in the in-phase linear ac susceptibility χ′(T) were observed, indicative of the magnetic glass transition at T_g∼60 K. Strongly divergent zero-field-cooled and field-cooled static magnetizations and frequency dependent ac susceptibility are evident of the glassy-like magnetic state of the compound at low temperatures. The frequency dependence of the cusp temperature T_max of the χ′(T) susceptibility was found to follow the critical slowing down mechanism. The Cole–Cole analysis of the dynamic susceptibility at low temperature has shown extremely broad distribution of relaxation times, indicating that spins are frozen at “macroscopic” time scale. Slow relaxation in the zero-field-cooled magnetization has been experimentally revealed. The obtained results do not agree with a canonical spin-glass state and indicate a cluster glass magnetic state of the compound below T_g, associated with its antiferromagnetic–ferromagnetic nano-phase segregated state. It was found that the relaxation mechanisms below the cluster glass freezing temperature T_g and above it are strongly different. Magnetic field up to about μ₀H∼0.4 T suppresses the glassy magnetic state of the compound.     

Viscous behavior in a quasi-1D fractal cluster glass

The spin glass transition of a quasi-1D organic-based magnet ([MnTPP][TCNE]) is explored using both ac and dc measurements. A scaling analysis of the ac susceptibility shows a spin glass transition near 4 K, with a viscous decay of the thermoremanent magnetization recorded above 4 K. We propose an extension to a fractal cluster model of spin glasses that determines the dimension of the spin clusters (D) ranging from approximately 0.8 to over 1.5 as the glass transition is approached. Long-range dipolar interactions are suggested as the origin of this low value for the apparent lower critical dimension.     

Formation and partial melting of two types of spin-cluster glass behavior in vanadate spinel

We report the doping effect on the various properties of spinels Co(1-x)Zn(x)V(2)O(4) (0 ≤ x ≤ 0.2). For the parent compounds, the rise in magnetization, the valley in thermal conductance, the transition from the ferromagnetic arrangement to non-collinear alignment indicated by the specific heat for the V sublattice, especially the frequency dependence of AC susceptibility around T(1) = 59 K, verify the occurrence of the transition at T(1) besides the ferrimagnetic transition at T(C). The ferrimagnetic transition at T(C) induces the spin-cluster glass behavior and the transition at T(1) yields the new spin-cluster glass (NSCG) behavior. As the Zn(2+)-doped content increases, the above phenomena are gradually weakening to vanishing, but the glassy behavior at T(C) still exists for all samples. Through the fourth-order perturbation theory, we discuss the reasons for the gradual vanishing of the transition at T(1).     

Cluster spin glass and superparamagnetism in RuSr<Subscript>2</Subscript>Eu<Subscript>1.5</Subscript>Ce<Subscript>0.5</Subscript>Cu<Subscript>2</Subscript>O<Subscript>10-</Subscript><Subscript>δ</Subscript>

We investigate in detail the dc magnetization and nonlinear ac susceptibility behavior of the superconducting ferromagnet RuSr₂Eu_1.5Ce_0.5Cu₂O_{10- δ} (Ru1222) to develop a comprehensive understanding of the spin glass and superparamagnetism in this material. The structural properties of the system result in the formation of magnetic (ferromagnetic) clusters of different sizes, shapes and properties. The magnetic clustering of the system leads to observation of various features in dc magnetization and ac susceptibility consistent with superparamagnetism and cluster spin glass states, which can coexist or stand alone, depending on the temperature range considered. Experimental results of magnetic measurements in combination with their analysis have enabled us to explain and distinguish these phenomena, as well as to propose a temperature dependent scenario of the system behavior.     

Correlation between reentrant spin glass behavior and the magnetic order-disorder transition of the martensite phase in Ni-Co-Mn-Sb Heusler alloys

We have performed ac susceptibility and dc magnetization measurements in Ni(50-x)Co(x)Mn(38)Sb(12) Heusler alloys. From the ac susceptibility measurements, the existence of reentrant spin glass (RSG) state is observed for x=0-5. It is found that the signature of RSG behavior diminishes with increase in x. This behavior is in contrast to the fact that the exchange bias field increases with x, which reveals that the origins of RSG and exchange bias are different in the present system. It is found that the system enters a frustrated ferromagnetic state just below the Curie temperature of the martensite phase (T(M)(C)) and then the RSG state at low temperature. The strength of the RSG state is critically dependent on the sharpness of the magnetic transition at (T(M)(C)). This proposition is further supported by the thermo-remanent magnetization and low field thermomagnetic measurements.     

Relaxation phenomena in ensembles of CoFe2O4 nanoparticles

Collective magnetic behavior of CoFe₂O₄ nanoparticles with diameters of 76, 16, 15 and 8 nm, respectively, prepared by different chemical methods has been investigated. Particle composition, size and structure have been characterized by inductive coupled plasma (ICP), transmission electron microscopy (TEM) and powder X-ray diffraction (PXRD). Basic magnetic properties have been determined from the temperature dependence of magnetization and magnetization isotherms measurements. The three samples exhibit characteristic of a superparamagnetic system with the presence of strong interparticle interactions. Magnetic relaxation phenomena have been examined via frequency-dependent ac susceptibility measurements and aging and memory effect experiments. For the particles coated with oleic acid, it has been demonstrated that the sample reveals all attributes of a super-spin glass (SSG) system with strong interparticle interactions.     

Cluster spin glass ordering in diluted spinel Zn0.5Co0.5FeCrO4

The disordered spinel system, Zn_0.5Co_0.5FeCrO₄ has been investigated using the low field magnetization and ac susceptibility measurements. From the present results it appears that this system orders into a cluster spin glass state with the magnetic moments of the ferrimagnetic clusters randomly frozen. Compared to the Ni and Co zinc ferrites with the same magnetic dilution, introduction of Cr into the B sites appears to increase the frustration and disorder dramatically. The predicted phase diagrams for the ordering in diluted magnetic spinels do not describe the magnetic behaviour of this system, presumably due to the disorder in the B sublattice in addition to the dilution in the A sublattice.     

The role of iron in the formation of the magnetic structure and related properties of La0.8Sr0.2Co1−xFexO3 (x=0.15, 0.2, 0.3)

La_0.8Sr_0.2Co_1−xFe_xO₃ (x=0.15, 0.2, 0.3) samples were studied by means of AC magnetic susceptibility, magnetization, magnetoresistance and ⁵⁷Fe Mössbauer spectrometry. Iron was found to take on a high spin 3d^5−α electronic state in each of the samples, where α refers to a partly delocalized 3d electron. The compounds were found to exhibit a spin-cluster glass transition with a common transition temperature of ∼53 K. The spin-cluster glass transition is visualized in the ⁵⁷Fe Mössbauer spectra as the slowing down of magnetic relaxation below ∼70 K, thereby showing that iron takes part in the formation of the glassy magnetic phase. The paramagnetic-like phase found at higher temperatures is identified below T_c≈195 K as being composed of weakly interacting, magnetically ordered nanosized clusters of magnetic ions in part with a magnetic moment oriented opposite to the net magnetic moment of the cluster. For each of the samples a considerable low-temperature negative magnetoresistance was found, whose magnitude in the studied range decreases with increasing iron concentration. The observed results obtained on the present compounds are qualitatively explained assuming that the absolute strengths of magnetic exchange interactions are subject to the relation ∣J_Co–Co∣<∣J_Fe–Co∣<∣J_Fe–Fe∣.     

Magnetite (Fe3O4): a new variant of relaxor multiferroic?

The electric polarization, dielectric permittivity, magnetoelectric effect, heat capacity, magnetization and ac susceptibility of magnetite films and polycrystals were investigated. The electric polarization of magnetite films with saturation values between 4 and 8 μC cm(-2) was found to vanish between 32 and 38 K, but in polycrystals no phase transition was detected in this range by heat capacity. Both types of samples showed magnetoelectric effects at low temperatures below a frequency-dependent crossover. This is interpreted as arising from multiferroic relaxor behavior.     

Magnetic order in hybrid frustrated magnets Gd(2-x)Tb(x)Ti2O7 (x = 0.2 and 0.5)

We report on the specific heat, magnetization and ac susceptibility measurements of single crystals of hybrid frustrated magnets Gd(1.8)Tb(0.2)Ti(2)O(7) and Gd(1.5)Tb(0.5)Ti(2)O(7). The analysis of experimental data revealed that, although partial replacing of the Gd(3+) ions by the Tb(3+) ions in the Gd(2)Ti(2)O(7) host lattice slightly enhances antiferromagnetic coupling, as inferred from the evolution of the paramagnetic Curie-Weiss temperature, the ordering temperature gradually decreases. Paramagnetic correlations introduced by the Tb(3+) ions cause this perturbation, altering the effective further neighbor interactions and destabilizing the ground state in Gd(2)Ti(2)O(7). In addition, the low-energy states of Gd(2-x)Tb(x)Ti(2)O(7) are suggested to possess a nature different from those in parent members Tb(2)Ti(2)O(7) and Gd(2)Ti(2)O(7). Finally, the frequency-dependent magnetic susceptibility behavior in Gd(1.5)Tb(0.5)Ti(2)O(7) is consistent with the formation of a spin-glass-like state indicating a pronounced slowing down of the dynamical response of the studied hybrid magnets.     

Reentrant spin glass behaviour in Nd0.84K0.12MnO3

Polycrystalline Nd_0.84K_0.12MnO₃ was prepared in single phase form with Pbnm space group. The magnetic properties are studied from magnetization, linear and non-linear susceptibility, and thermoremanent magnetization measurements. The sample exhibits paramagnetic to ferromagnetic transition followed by low temperature spin glass like transition. From frequency variation of ac susceptibility measurements, the spin glass transition temperature is found to be 97.6±0.1 K with critical exponents zυ=1.13±0.06. The critical exponent γ corresponding to spin glass transition has been determined from the third harmonic susceptibility analysis and it is found to be 3.09±0.05. The effective number of spins blocked under frustration and their correlation length are determined from the analysis of thermoremanent magnetization.     

Effective mass enhancement and spin-glass behaviour in CeCu4Mn(y)Al(1-y) compounds

We report on the magnetic ac/dc susceptibility and specific heat measurements for the CeCu(4)Mn(y)Al(1-y) series of compounds with 0 ≤ y ≤ 1. All compounds investigated crystallize in the hexagonal CaCu(5)-type structure with the space group P6/mmm. The results reveal that the frustration of the interactions dominates and leads to a spin-glass (SG) behaviour with a linear change of the freezing temperature T(f) as a function of y. The SG state has been confirmed by the frequency dependence of the ac magnetic susceptibility, the relaxation of the remanent magnetization and the split of the field-cooled-zero-field-cooled dc magnetic susceptibility. The electronic specific heat coefficient γ is enhanced for all y and increases with the Al content. Below a threshold at y ≈ 0.3, γ is large even if determined for temperatures above T(f); moreover the paramagnetic Curie-Weiss temperature θ(p) changes sign to negative. These observations indicate the possible presence of the heavy fermion (HF) state, at least below y ≈ 0.3, and the possible coexistence of the SG and HF states down to y = 0, i.e. for the CeCu(4)Al compound. A tentative magnetic phase diagram for CeCu(4)Mn(y)Al(1-y) has been constructed.     

Spin dynamics of the S = 5/2 2D triangular antiferromagnet Ba3NbFe3Si2O14

We report pulse-field magnetization, ac susceptibility, and 100 GHz electron spin resonance (ESR) measurements on the S = 5/2 two-dimensional triangular compound Ba3NbFe3Si2O14 with the Néel temperature T(N) = 26 K. The magnetization curve shows an almost linear increase up to 60 T with no indication of a one-third magnetization plateau. An unusually large frequency dependence of the ac susceptibility in the temperature range of T = 20-100 K reveals a spin-glass behavior or superparamagnetism, signaling the presence of frustration-related slow magnetic fluctuations. The temperature dependence of the ESR linewidth exhibits two distinct critical regimes; (i) ΔH(pp)(T) is proportional to (T-T(N))(-p) with the exponent p = 0.2(1)-0.2(3) for temperatures above 27 K, and (ii) ΔH(pp)(T) is proportional to (T-T*)(-p) with T* = 12 K and p = 0.8(1)-0.8(4) for temperatures between 12 and 27 K. This is interpreted as indicating a dimensional crossover of magnetic interactions and the persistence of short-range correlations with a helically ordered state.     

Coexistence of spin glass and antiferromagnetic orders in Ba3Fe2.15W0.85O8.72

Ba(3)Fe(2.15)W(0.85)O(8.72) has been grown as large single crystals using the floating-zone method, permitting very precise characterization of the nuclear and magnetic structures by neutron and synchrotron diffraction methods. The results of our structural investigation are combined with dc and ac magnetization and heat capacity measurements to give an unusually complete and detailed picture of a complex magnetic system. The compound crystallizes in the hexagonal perovskite structure (space group P6(3)/mmc) and reveals antiferromagnetic order below T(N) = 290 K. Frequency-dependent ac susceptibility and the presence of magnetic viscosity suggest the onset of a spin glass component in this material below T(f) = 60 K. These findings are discussed on the basis of detailed analysis of the crystalo-chemical properties, supported by ab initio (density functional theory) calculations.     

Spin disorder induced reentrant ferromagnetism in iron-based nanocomposites

The low-temperature magnetic behavior of pure iron nanocrystallites dispersed in MgO matrix has been investigated by dc magnetization and ac susceptibility measurements. Irreversibilities in the magnetization data at low field are observed at low temperatures, indicating a passage from a high temperature ferromagnetic phase to a low-temperature disordered, frozen state. Quenching of these irreversibilities is seen when the external magnetic field is increased. The variation of the in-phase susceptibility with temperature showed marked frequency dependence whereas the out-of-phase susceptibility component passes through a maximum. The origin of this behavior is traced to the spin disorder at the grain boundaries, which exhibit a co-operative freezing below a certain temperature.     

Double peaks on ac magnetization in a superconducting Pb-porous glass nanocomposite

Studies of temperature dependences of ac magnetization were carried out for a superconducting lead-porous glass nanocomposite. Double peaks were found on the imaginary part of ac magnetization which were accompanied with double steps on the real part. The lower-temperature anomalies in ac magnetization differed noticeably when they were obtained upon cooling and warming. The double peaks were treated as two phase transitions in the vortex system: the liquid-solid transition which occurs close to the onset of superconductivity and solid-solid one which is triggered by superconductivity in confined lead islands.     

57Fe Mössbauer spectroscopy on the cyclic spin-cluster Fe6(tea)6(CH3OH)6

We present ⁵⁷Fe Mössbauer spectroscopy experiments on the cyclic spin-cluster Fe₆(tea)₆(CH₃OH)₆ (tea = triethanolaminato(-3)). In former studies, the spin cluster has been treated as a homogenous, quasi-one-dimensional spin S=5/2 Heisenberg antiferromagnet. Our experiments reveal spectra, which consists of two different quadrupolar doublets. In consequence, there are two different Fe sites among the hexanuclear iron spin-cluster.     

Magnetic study of CaMn0.96Mo0.04O3, canting vs. phase separation

CaMn_0.96Mo_0.04O₃ is an example of Mn⁴⁺ rich perovskite manganites, which exhibits a net ferromagnetic component at low temperature, observed by dc magnetization and ac susceptibility. To characterize the magnetic state of this compound, neutron powder diffraction was carried out in the 2-400 K temperature range, showing that it is necessary to use three components (ferromagnetic and G- and A-type antiferromagnetic) to describe it. This particular state is in agreement with the unusual magnetic behaviour observed by macroscopic measurements and is compared to the one observed for manganites with similar Mn valence but obtained by A-site substitution.     

Evidence for strain glass in the ferroelastic-martensitic system Ti(50-x)Ni(50+x)

We report here "strain glass," a new glassy phenomenon in ferroelastic-martensitic system of Ni-rich intermetallic Ti(50-x)Ni(50+x) (x > 1), where local strain is frozen in disordered configuration below a critical temperature Tg. The ac elastic modulus shows a minimum at Tg, which exhibits logarithmic frequency dependence following Vogel-Fulcher relationship, and the corresponding internal friction shows a frequency-dependent peak located at a lower temperature. In situ high-resolution transmission electron microscopy observations reveal uncorrelated nanoclusters of martensiticlike phase, randomly frozen in the otherwise untransformed parentlike matrix. Being parallel to spin glass and relaxor, strain glass may shed new light on the fundamental physics of glass and lead to the discovery of novel properties.