Effects of Fe doping on ac susceptibility of Pr0.75Na0.25MnO3

Ac susceptibility at low temperatures of Pr_0.75Na_0.25Mn_1-xFe_xO₃ (0 ≤ x ≤ 0.30) is investigated. The peak value of the real component of ac susceptibility χ' at the freezing temperature T_f is suppressed with the increasing frequency. The peak value of χ' shows a linear relation between T_f and the logarithm of the frequency ω. The normalized slope P = ΔT_f/T_fΔlgω, which is much lower than canonical insulating spin glass systems in which 0.06 ≤ P ≤ 0.08. The peak value of the imaginary component of the ac susceptibility χ' at T_f for the x = 0, 0.02, 0.30 samples increases with increasing frequency, suggesting a cluster glass ground state with a coexistence of charge-ordered phase and correlated ferromagnetic clusters in spin glass matrix. The peak value of χ' at T_f for the x = 0.10 sample decreases with increasing frequency, suggesting a phase separation ground state. The peak value of χ' at T_f for the x = 0.05 sample decreases with increasing frequency for ω ≤ 52 Hz and increases subsequently till 701 Hz, and then decreases with further increasing frequency for ω ≥ 1501 Hz. This complex behaviour is ascribed to the competition between the effects of large and little ferromagnetic clusters in the sample. The ground state of x = 0.05 sample is a transition state from cluster glass to phase separation.     

Magnetic phase coexistence in Tb- and Sr-doped La0.7Ca0.3MnO3 manganite:A temperature-dependent neutron diffraction study

We report the results of the temperature-dependent neutron diffraction measurements on the nearly half-doped (La_0.325Tb_0.125)(Ca_0.3Sr_0.25)MnO₃ manganite sample. The simultaneous doping of magnetic Tb³⁺ and divalent Sr²⁺ in the La_0.7Ca_0.3MnO₃ system results into a large A-site size disorder. Rietveld refinement of neutron diffraction data reveal that the single phase sample crystallizes in a distorted orthorhombic structure. Increased 〈r_A〉 value affects the transport behavior that results into an insulating-like behavior of the sample. Under application of 1 T field sample exhibit insulating-like behavior while insulator-metal transition (T_IM) is exhibited under 5 and 8 T fields. Variable range hoping (VRH) mechanism of charge carriers is exhibited in the insulating region. Field cooled and zero field cooled magnetization measurement shows the Curie temperature (T_C)~47 K. The refinement of the ND data collected at various temperatures below 300 K shows that there is no structural phase transition in the compound. Around 100 K, a magnetic peak appears at lower angle that can be ascribed to the presence of the A-type antiferromagnetic (AFM) phase. Two more peaks are observed around 50 K at lower angles that can be fitted in CE-type antiferromagnetic phase. Splitting of the peaks at lower temperatures is the signature of orbital ordering in the presently studied nearly half-doped manganite system. Results of the detailed structural analysis of the temperature-dependent ND measurements on (LaTb)_0.45(CaSr)_0.55MnO₃ sample has been discussed in the light of coexisting A-type and CE-type antiferromagnetic phases present in the sample at low temperature.     

Effect of surface-topology on magnetic properties in (La0.6Eu0.4)0.67Ca0.33MnO3 of anisotropic shape of nanoplates

(La_0.6Eu_0.4)_0.67Ca_0.33MnO₃ has been prepared in the shape of nanoplates of single crystallites (an orthorhombic structure) through polymer templates. HRTEM images reveal 18, 25, and 30 nm thicknesses of plates after heating a precursor powder at 873, 1073, and 1273 K in air for 2 h. These values present average crystallite size determined from broadening of the X-ray diffraction peaks. A spin-glass-like surface (GS) overlayer (3-5 nm thickness) in such plates facilitates a ferromagnetic→ferrimagnetic reordering with markedly suppressed Curie point T_C, i.e., as small as 90 K in a 873 K heated sample, from the parent value 268 K. The T_C point increases to 103 K (or 120 K) when heating at higher temperature 1073 (or 1273 K), during which the core grows at the expense of the overlayer. The GS tailors as high coercivity H_c as 617 Oe in the zero field cooled (ZFC) sample that is decreased to 500 Oe in the field cooled (FC) sample in the surface spin-freezing along the field direction. The H_c-value (ZFC) that steps down successively to 252 Oe on the overlayer is thinned down by heating at 1273 K. Samples heated at 873, 1073, or 1273 K have regularly increased saturation magnetization 35.3, 63.9, or 69.6 emu/g in ZFC, while 43.7, 70.2, or 75.5 emu/g in FC measured at 10 K. The ferrimagnetic reordering are described based on the scenario of an antiferromagnetic exchange coupling between the Eu³⁺ and Mn³⁺ (or Mn⁴⁺) sublattices.     

Surface spin-glass-like behavior of monodispersed superparamagnetic Mn0.5Zn0.5Fe2O4 magnetic fluid

Zero field cooled dc-magnetization measurements of monodispersed Mn_0.5Zn_0.5Fe₂O₄ nanoparticles dispersed in kerosene exhibit two transitions at low temperatures. These transitions correspond to (i) the superparamagnetic to blocked superparamagnetic and (ii) the blocked superparamagnetic to surface spin-glass like/quantum superparamagnetic state upon lowering the temperature. The existence of a disorder surface is confirmed by recording small-angle neutron scattering data below and above the Curie temperature. Magnetic relaxation analysis shows a plateau at low temperature (below 5 K) with a slight minimum at 3 K, which is a characteristic of the surface spin-glass-like state. This is analyzed considering the energy distribution n(E)∼1/E. The existence of surface disorder dominates at low temperature and mimics the transition from superparamagnetic to quantum superparamagnetic states.     

Electrical and magnetic properties of ε-Fe3N nanoparticles synthesized by chemical vapor condensation process

ε-Fe₃N nanoparticles synthesized by chemical vapor condensation (CVC) are covered with shells of disordered Fe₃O₄ phase, as observed by a transmission electron microscopy. The zero-field cooling and field cooling temperature dependence of magnetization, ac susceptibility as a function of frequency, magnetic hysteresis loops, and the temperature dependence of resistivity of the ε-Fe₃N nanoparticles are systematically studied. The results indicate the existence of complex magnetic properties, such as superparamagnetic behavior, exchange bias, magnetic dipole interaction, and the possible coexistence of ferromagnetic and spin-glass-like states and/or disordered surface spins of the shells at low temperatures. The temperature dependence of resistivity ρ(T) for compacted ε-Fe₃N nanoparticles in a temperature range of 110 K< T< 300 K can be well described by the mechanism of fluctuation-induced tunneling conduction, while that below 110 K can be ascribed to conducting electrons scattered by localized magnetic moments and impurity as well as the influence of freezing of spin-glass-like moments and/or disordered surface spins of the shells.     

Spin-glass-like behaviour and magnetic order in Mn[Cr0.5Ga1.5]S4 spinels

Magnetization and susceptibility were investigated as a function of temperature and magnetic field in polycrystalline Mn[Cr_0.5Ga_1.5]S₄ spinel. The dc susceptibility measurements at 919 Oe showed a disordered ferrimagnetic behaviour with a Curie-Weiss temperature θ_CW=−55 K and an effective magnetic moment of 5.96 μ_B close to the spin-only value of 6.52 μ_B for Cr³⁺ and Mn²⁺ ions in the 3d³ and 3d⁵ configurations, respectively. The magnetization measured at 100 Oe revealed the multiple magnetic transitions with a sharp maximum at the Néel temperature T_N=3.9 K, a minimum at the Yafet-Kittel temperature T_YK=5 K, a broad maximum at the freezing temperature T_f=7.9 K, and an inflection point at the Curie temperature T_C=48 K indicating a transition to paramagnetic phase. A large splitting between the zero-field-cooled (ZFC) and field-cooled (FC) magnetizations at a temperature smaller than T_C suggests the presence of spin-glass-like behaviour. This behaviour is considered in a framework of competing interactions between the antiferromagnetic ordering of the A(Mn) sublattice and the ferromagnetic ordering of the B(Cr) sublattice.     

Detection of structural and magnetic transitions in La0.67Ba0.23Ca0.1MnO3 using the rf resonance technique

We report radio-frequency (rf) electrodynamics in polycrystalline La_0.67Ba_0.23Ca_0.1MnO₃ as a function of temperature and magnetic field using a home-built LC resonant circuit powered by an integrated chip oscillator. The resonance frequency (f_r) of the oscillator and the power (P) absorbed by the sample are measured simultaneously. The paramagnetic to ferromagnetic phase transition in the absence of an external magnetic field is accompanied by a rapid decrease in both P and f_r around the Curie temperature T_C=300 K. However, much below T_C, the f_r shows a step-like anomaly around 165 K (195 K) while cooling (warming), which we attribute to a structural phase transition from high temperature rhombohedral () to low temperature orthorhombic (Imma) phase. The step-like anomaly in f_r versus T disappears in a field of 300 G. Fractional changes as large as 19% in Δf_r/f_r and 10% in ΔP/P are observed under H=1 kG around T_C. Our study suggests that the rf resonance technique is a versatile tool to study the magnetization dynamics as well as to investigate the structural phase transition in manganites.     

Spin glass like behavior in Cd0.42Mn0.58In2S4

The magnetic behavior of the diluted magnetic semiconductor Cd_0.42Mn_0.58In₂S₄ has been study by dc magnetization and ac susceptibility experiments. Zero field cooled and field cooled measurements reveal irreversibility below T_irr=2.60±0.15 K. Ac susceptibility data, performed as a function of the temperature and the frequency, confirm the spin-glass like behavior of the material with T_f=2.75±0.15 K. High temperature susceptibility data follow a typical Curie-Weiss law with θ=−74±1 K which suggests predominant antiferromagnetic interactions. The randomness of the magnetic ions, necessary to explain the magnetic behavior of the material, has been determined by X-ray powder diffraction experiments.     

Influence of spin-glass-like phase on magnetic and electrical transport properties of reactive sputtered Al1−xFexN films

Nanocrystalline Al_1−xFe_xN films were fabricated using the reactive sputtering method. A large amount of spin-glass-like moments are in the films. With the decrease of temperature, the films turn from the spin-glass-like behavior to ferromagnetism. At low temperatures, the saturation magnetization increases and the coercivity decreases with the increase of x. The coercivity increases significantly below 50 K due to the pinning effect of the frozen disordered spin-glass-like moments. All of the films are semiconducting. The low-temperature transport mechanism turns from tunneling to hopping as x increases. Magnetoresistance (MR) shows weak saturation trend with the applied field because of the hard alignment of the frozen moments. Meanwhile, MR follows the relation of log |MR|=a+bT−1, and the spin polarization satisfies P(T)=P₀e−βTα, related with the disordered spin-glass-like moments.     

Probing the magnetic state by linear and non-linear ac magnetic susceptibility measurements in under-doped manganite Nd0.8Sr0.2MnO3

We have thoroughly investigated the entire magnetic states of under-doped ferromagnetic-insulating manganite Nd_0.8Sr_0.2MnO₃ through temperature-dependent linear and non-linear complex ac magnetic susceptibility measurements. This ferromagnetic-insulating manganite is found to have frequency-independent ferromagnetic to paramagnetic transition temperature at around 140 K. At around 90 K (≈T_?) the sample shows a second frequency-dependent re-entrant magnetic transition as explored through complex ac susceptibility measurements. Non-linear ac susceptibility measurements (higher harmonics of ac susceptibility) have also been performed (with and without the superposition of a dc magnetic field) to further investigate the origin of this frequency dependence (dynamic behavior at this re-entrant magnetic transition). Divergence of 3rd harmonic of ac susceptibility in the limit of zero exciting field indicates a spin-glass-like freezing phenomena. However, large value of spin-relaxation time (τ₀=10⁻⁸ s) and small value of coercivity (∼22 Oe) obtained at low temperature (below T_?) from critical slowing down model and dc magnetic measurements, respectively, are in contrast with what generally observed in a canonical spin glass (τ₀=10⁻¹²-10⁻¹⁴ s and very large value of coercivity below freezing temperature). We have attributed our observation to the formation of finite size ferromagnetic clusters which are formed as consequence of intrinsic phase separation and undergo cluster glass-like freezing below certain temperature in this under-doped manganite. The results are supported by the electronic- and magneto-transport data.     

The superparamagnetic response of a Co54Ga46 alloy to low d.c. fields

The low d.c. field susceptibilities and thermoremanence of a Co₅₄Ga₄₆ alloy are presented. A broad peak is observed in the zero field cooled susceptibility at a temperature T_B, which decreases with increasing magnetic field, while the thermoremanence is found to persist to temperatures greater than T_B. The behaviour is discussed in terms of the growth and subsequent blocking of superparamagnetic assemblies.     

A novel double-peaked spin-glass susceptibility-temperature response in the ternary alloy Fe69Mn26Cr5

We have studied the low-field (B ≦ 10^?2 T) d.c. susceptibility χ of the austenitic stainless-steel alloy Fe₆₉Mn₂₆Cr₅ as a function of the magnetic field B and temperature T. χ(T) shows structure, strong B dependence, and typical irreversible effects. The range of temperatures studied comprises three distinct regions. In the high-temperature region (300 K ≦ T ≦ 380 K) a blunt peak in the susceptibility is noticed at T₂ = 340 K. T₂ was not sensitive to thermal cycling. χ(T) displayed a sharp cusp at T₁ = 200 K. This peak was sensitive to the thermal history of the sample and was strongly suppressed by B. Between T₁ and T₂ a shallow valley with some hysteresis was observed. We interpret this behavior to be due to a low-temperature pure spin-glass phase, a high temperature conventional paramagnetic phase, and coexisting antiferromagnetic and spin-glass phases between T₁ and T₂.     

Spin-glass-like phase behaviour in CeNi2−xCuxSn2

We report the results of our investigation in CeNi_2−xCu_xSn₂ (x=0, 0.4, 1.0, 1.6 and 2.0), a new pseudoternary series with CaBe₂Ge₂-type tetragonal structure. Substitution of Cu for Ni leads to a linear increase in the constants a, c and the unit cell volume v. As probed by the low temperature dependence of ac susceptibility χ_ac(T), the T_f temperature, which corresponds to the freezing temperature of the spin-glass clusters, is annihilated above 2.0 K significantly for the samples with x≥1.6. This observation proves conclusively that the Ni-rich samples in the series CeNi_2−xCu_xSn₂ have the advantage of forming the spin-glass-like state.     

Spin-glass-like behavior in ZnxCryAlzSe4

The magnetic and electrical properties of the Al-doped polycrystalline spinels Zn_xCr_yAl_zSe₄ (0.13≤z≤0.55) with the antiferromagnetic (AFM) order and semiconducting behavior were investigated. A complex antiferromagnetic structure below a Néel temperature T_N≈23 K for the samples with z up to 0.4 contrasting with the strong ferromagnetic (FM) interactions evidenced by a large positive Curie-Weiss temperature θ_CW decreasing from 62.2 K for z=0.13 to 37.5 K for z=0.55 was observed. Detailed investigations revealed a divergence between the zero-field-cooling (ZFC) and field-cooling (FC) susceptibilities at temperature less than T_N suggesting bond frustration due to competing ferromagnetic and antiferromagnetic exchange interactions in the compositional range 0.13≤z≤0.4. Meanwhile, for z=0.55 a spin-glass-like behavior of cluster type with randomly oriented magnetic moments is observed as the ZFC-FC splitting goes up to the freezing temperature T_f=11.5 K and the critical fields connected both with a transformation of the antiferromagnetic spin spiral via conical magnetic structure into ferromagnetic phase disappear.     

Magnetodielectric coupling in MnCr2O4 spinel

We have investigated the magnetic and dielectric properties of polycrystalline samples of the spinel MnCr₂O₄. Below the ferrimagnetic ordering temperature at T_N∼43 K, both magnetization and dielectric measurements show signatures of the onset of a conical structure at T_s∼17 K and a lock-in temperature at T_f∼14 K. These values are similar to those previously reported for single-crystal samples, where the spiral structure is short-range ordered (SRO) at low temperatures. The application of magnetic field suppresses the dielectric anomaly at T_f indicating that the coherence length of the ordering increases. MnCr₂O₄ exhibits a symmetrical magnetodielectric response between T_f and T_s that scales with the square of the magnetization. This suggests that the magnetodielectric coupling originates from the P²M² term in the free energy expansion. The magnetodielectric response becomes asymmetric with respect to field below T_f.     

Low-frequency alternative-current magnetic susceptibility of amorphous and nanocrystalline Co60Fe20B20 films

This investigation experimentally studies the low-frequency alternating-current magnetic susceptibility (χ_ac) of amorphous and nanocrystalline CoFeB films by measuring the magnetic field established by passing currents of various frequencies through such films of various thicknesses (t_f). A CoFeB film is sputtered onto a glass substrate with t_f from 100 Å to 500 Å under the following conditions: (a) As-deposited films were maintained at room temperature (RT) and (b) films were post-annealed at T_A=150 °C for 1 h. The samples thus obtained are analyzed in a magnetic field that was generated by an alternating current (AC) at various frequencies from 10 Hz to 25,000 Hz. The experimental results demonstrate that the χ_ac declines as the thickness of the as-deposited sample and the post-annealed sample (T_A=150 °C) increases because the lower coercivity (H_c) of thinner CoFeB films is similar to a soft magnetic characteristic and is associated with a higher χ_ac value. The best χ_ac value is obtained at a thickness of 100 Å under both conditions. The χ_ac value of the post-annealed sample exceeds that of the RT sample at thicknesses from 100 Å to 500 Å because the magneto crystalline anisotropy of the post-annealed sample yields the highest χ_ac value at the optimal resonance frequency (f_res), at which the spin sensitivity is maximal. The X-ray diffraction patterns (XRD) of as-deposited CoFeB films reveal their amorphous structure. The XRD results for the post-annealed films include a main peak at 2θ=44.7° from the body-centered cubic (BCC) nanocrystalline CoFe that indicated a (110) textured structure. Post-annealing treatment caused that the amorphous structure to become more crystalline by a thermally driven process, such that the χ_ac value of the post-annealed sample exceeded that of the RT sample. This experimental result demonstrates that the χ_ac value decreased as the thickness of the thin film increased. Finally, the CoFeB thin films had the best χ_ac at low frequency (<50 Hz) following post-annealing treatment. The results obtained under the two conditions indicate that the maximum χ_ac value and the optimal f_res of a 100 Å-thick CoFeB thin film were 1.6 and 30 Hz, respectively, following post-annealing at T_A=150 °C for 1 h, suggesting that a 100 Å-thick CoFeB thin film that has been post-annealed at T_A=150 °C can be utilized as a gage sensor and in transformer applications at low frequencies.     

Room temperature ferromagnetism and magnetotransport properties of the layered manganite system La1.2Ba1.8Mn2−xRuxO7 (0≤x≤1.0)

The dc magnetization and ac susceptibility measurements on two dimensional layered manganite La_1.2Ba_1.8Mn₂O₇ samples reveal the occurrence of ferromagnetism above room temperature with ferromagnetic (FM) to paramagnetic (PM) transitions at 338 K. The bifurcation temperatures shown by the zero-field cooled (ZFC) and field cooled (FC) dc magnetization curves at high temperatures shift towards lower temperatures as the applied field is increased from 100 to 2500 Oe. The data are suggestive of a large magnetic anisotropy due to the strong competing ferromagnetic and antiferromagnetic interactions resulting in a spin-glass-like state. Ru doping is found to enhance the ferromagnetism and metallicity of the system in a remarkable way. The magnetoresistance (MR) values obtained are very high and about 40% even at 260 K for the undoped sample.     

Low field magnetoresistance and conduction noise in layered manganite La1.4Ca1.6Mn2O7

Temperature dependence of conduction noise and low field magnetoresistance of layered manganite La_1.4Ca_1.6Mn₂O₇ (DLCMO) are reported and compared with the infinite layered manganite La_0.7Ca_0.3MnO₃ (LCMO). The double layered manganite was prepared using standard solid state reaction method and had a metal-insulator transition temperature (T_M-I) of 155 K. The temperature dependence of susceptibility showed evolution of ferromagnetic ordering at 168 K. The observed voltage noise spectral density (S_V) shows 1/f^α type of behaviour at all temperatures from 77 K to 300 K. In the ferromagnetic region (T<168 K), S_V/V² shows two peaks at 164 K and 114 K. The observed two peaks in normalised conduction noise of DLCMO is attributed to the excess noise generated due to setting up of short range 2D-ferromagnetic ordering and long range 3D-ferromagnetic ordering at two different temperatures T_C2 and T_C1. In temperature range between T_C1 and T_C2, the magnetoresistance (MR) showed a gradual increase with the magnetic field. The observed MR has been explained in the framework of the two phase model [ferromagnetic (FM) domains and paramagnetic (PM) regions].     

Neutron scattering studies of the reentrant spin-glass system PdFeMn

Small angle neutron scattering (SANS) and inelastic neutron scattering studies were performed on a polycrystalline sample of (Pd_{9 9.65}Fe_0.35)₉₅Mn₅. This system exhibits a sequence of phase transitions from a paramagnetic to ferromagnetic state and then a transition to spin-glass-like behavior near T_SG = 3.0 K. The temperature dependence of the SANS exhibits a peak at T_c = 9.0 K and then a Q-dependent increase at low temperatures. This low temperature behavior contrasts sharply with that observed at low temperatures for a normal ferromagnet. No spin waves were observed within the ferromagnetic phase for the momenta values probed. Instead, a broad (FWHM ～ 5.0 meV) quasielastic distribution which was almost temperature independent was observed. This scattering was interpreted as a measure of the distribution of the magnetic energies of the Mn²⁺ ions.     

Ground-state magnetism of chromium-substituted LiMn2O4 spinel

Comparative crystal structure and magnetic properties studies have been conducted on quaternary powder spinel samples LiMn_1.82Cr_0.18O₄ obtained by two different synthesis methods, glycine-nitrate (GN) and ultrasonic spray-pyrolysis (SP). Although both samples possess the same spinel structure of the cubic space group Fd3¯m, their low-temperature magnetic properties display significant differences. While the SP sample undergoes only spin-glass transition at the freezing temperature T_f=20 K, the GN sample possesses more complicated low-temperature magnetic behavior of the reentrant spin-glass type with the Néel temperature T_N=42 K and freezing temperature T_f=22 K. High-temperature magnetic susceptibility of both samples is of the Curie–Weiss type with the effective magnetic moments in agreement with the nominal compositions. This fact together with the results of the chemical analysis discards the existence of the diversity in chemical compositions as a possible cause for the observed differences in the low-temperature magnetism. On the other hand, the crystal structure analysis done by the Rietveld refinement of the X-ray powder diffraction data points to the strong influence of the cation distribution on the ground-state magnetism of these systems. An explanation of this influence is proposed within the framework of a collective Jahn–Teller effect.