Hyperfine interactions in icosahedral quasicrystals: a Mössbauer study

Icosahedral Al₆₅Cu₂₀Fe₁₅ and Al₄₀Cu_9.9Ge₂₅Mn₂₅ ⁵⁷Fe_0.1 quasicrystals are studied using⁵⁷Fe transmission Mössbauer experiments. The spectra are analyzed by distributions of electric-quadrupole interaction accounting for line asymmetries. Temperature dependences of the hyperfine parameters derived comprising average values ofP() distributions, corresponding standard deviations and center shifts are presented in a whole range from 8 to 300 K.     

Structure and magnetic properties of FeMnAl alloys investigated by Mössbauer spectroscopy and X-ray diffraction

The system (Fe_0.88Mn_{0.12 1–x} Al _x has been investigated in a concentration range from 5 to 14 at.% Al. We applied Mössbauer spectroscopy in the temperature range from 4 up to 900 K and X-ray diffractometry at room temperature. The as-cast samples show a bcc phase for all concentrations and exhibit broadened six-line Mössbauer spectra typical for disordered alloys. The Mössbauer spectra during a high temperature treatment show dramatic changes. These are due to ordering processes appearing at temperatures above 700 K. As an example of the observed changes, we present results obtained for the alloy withx= 14 at.% Al.     

Spin glass ordering of Zn0.75Co0.25Fe0.5Cr1.5O4 cubic spinel

The linear and nonlinear low field AC susceptibilities of Zn_0.75Co_0.25Fe_0.5Cr_1.5O₄ show peaks due to non-critical contributions, which mask the peak due to spin glass ordering. They extend into the region of temperatures in which Mössbauer spectra do not show any magnetic component. When a DC field of 200 Oe suppresses the non-critical contributions, peak due to spin glass ordering is clearly visible. The spin glass ordering is thus shown to be a thermodynamic transition. The critical exponent is found to fall within the range found using other spin glasses. Mössbauer spectra in zero fields provide T_SG, which agrees with the peak temperature of AC susceptibilities in the absence of non-critical contributions. 〈S_Z〉 determined using Mössbauer spectra does not show any anomaly. In the presence of a field of 5 T, the spectra show SG ordering at 4.2 K, which converts into ferrimagnetic ordering at higher temperatures.     

Hyperfine field distribution in reentrant spin glass alloys

The hyperfine field distribution in reentrant spin glass alloys Cr-Fe and Fe₇₀Al₃₀ was obtained by means of Mössbauer absorption. For Cr-Fe, the distribution curves generally composed of double peaks but tend to form a single peak by lowering temperature. This fact indicates that the spin glass state appearing at low temperature is uniform. For Fe₇₀Al₃₀, the curves consist of three peaks at low temperature. This behavior is interpreted by considering the atomic order and the mechanism of the moment inducement in the alloy.     

Magnetic properties of nanocrystalline Ni0.7Mn0.3Gd0.1Fe1.9O4 ferrite at low temperatures

Mössbauer spectra and magnetic measurement of Ni_0.7Mn_0.3Gd_0.1Fe_1.9O₄ ferrite were investigated by Oxford MS-500 Mössbauer spectrometer and superconducting quantum interference device (SQUID) magnetometer with a field 5 T. Ni_0.7Mn_0.3Gd_0.1Fe_1.9O₄ nanoparticles have a considerable coercivity of 1040 Oe when the test temperature is reduced to 2 K. Mössbauer spectra show that Ni_0.7Mn_0.3Gd_0.1Fe_1.9O₄ nanoparticles exhibit superparamagnetism at room temperature and ferrimagnetism at 77 K.     

Mössbauer,X-ray diffraction and AC susceptibility studies on nanoparticles of zinc substituted magnesium ferrite

Nanoparticles of zinc substituted Mg-ferrite with compositions Mg_(1-x)Zn _x Fe₂O₄ (x = 0.15, 0.30 and 0.50) having particle sizes in the range 6.4 nm to 21.4 nm prepared by the co-precipitation method were characterized by ⁵⁷Fe Mössbauer spectroscopy, X-ray diffratometry and AC magnetic susceptibility measurements. Mössbauer measurements at room temperature and down to 20 K clearly indicate presence of superparamagnetic particles in all the samples. AC magnetic susceptibility data show lowering of blocking temperature with decrease of particle size. Superparamagnetic relaxation was observed for larger particle size in samples with higher Zn content, which is attributed to the weakening of A-B exchange interaction in ferrite lattice due to replacement of Fe^{3 +} in tetrahedral site by Zn^{2 +} ions.Received: 16 April 2004, Published online: 23 July 2004PACS: 75.50.Tt Fine-particle systems; nanocrystalline materials - 76.80. + y Mössbauer effect; other gamma-ray spectroscopy - 75.30.Cr Saturation moments and magnetic susceptibilitiesS. Das: Present address: Department of Physics, Jadavpur University, Kolkata - 700032, India     

Mössbauer and magnetic studies of orthorhombic FeSiO3

Magnetic properties of orthoferrosilite FeSiO₃ have been examined using susceptibility, magnetization measurements and Mössbauer spectroscopy. From magnetic and Mössbauer measurements, one obtains close values of the magnetic ordering temperature, T_N=39±1 K and T_N=41±1 K, respectively. The magnetic order is characterized by strong ferromagnetic coupling of Fe²⁺ moments within the ribbons and a weak antiferromagnetic coupling of the moments between adjacent ribbons. The 4.2 K Mössbauer spectra can be fitted with two different hyperfine magnetic fields H_hf=68 kOe and H_hf=314 kOe which can be assigned to Fe²⁺ in the octahedrally coordinated M1 and M2 sites, respectively, of the FeSiO₃ structure.     

Mössbauer spectroscopy studies of spin reorientations in amorphous and crystalline (Co0.2Fe0.8)72.5Si12.5B15 glass coated micro-wires

Thermo-gravimetric, differential scanning calorimetry and comprehensive ⁵⁷Fe Mössbauer spectroscopy studies of amorphous and crystalline ferromagnetic glass coated (Co_0.2Fe_0.8)_72.5Si_12.5B₁₅ micro-wires have been recorded. The Curie temperature of the amorphous phase is T_C(amorp) ∼730 K. The analysis of the Mössbauer spectra reveals that below 623 K the easy axis of the magnetization is axial-along the wires, and that a tangential or/and radial orientation occurs at higher temperatures. At 770 K, in the first 4 hours the Mössbauer spectrum exhibits a pure paramagnetic doublet. Crystallization and decomposition to predominantly α-Fe(Si) and Fe₂B occurs either by raising the temperature above 835 K or isothermally in time at lower temperatures. Annealing for a day at 770 K, leads to crystallization. In the crystalline material the magnetic moments have a complete random orientation. After cooling back to ambient temperature, both α-Fe(Si) and Fe₂B in the glass coated wire show pure axial magnetic orientation like in the original amorphous state. The observed spin reorientations are associated with changes in the stress induced by the glass coating.     

Local order of icosahedral quasicrystals studied by Mössbauer spectroscopy

Thermodynamically stable Al-Cu-Fe and Fe-doped ferromagnetic Al-Cu-Ge-Mn icosahedral quasicrystals are studied by⁵⁷Fe transmission Mössbauer spectroscopy and X-ray diffraction experiments. Al₆₅Cu₂₀Fe₁₅ quasicrystalline alloy was subjected to a mechanical grinding (MG) for up to 800 hours in a ball mill. Presence of the amorphous phase which co-exists with the quasicrystalline one is revealed in the early stage of MG. Mössbauer measurements were performed on icosahedral Al₄₀Cu_10–x Ge₂₅Mn₂₅Fe _x quasicrystal (x0.1; 3) in a temperature range from 10 K to 548 K. It was found that a magnetic transition occurs at about 30 K which is far belowT _c reported in the literature. It is concluded that AlGeMn ferromagnet which is present in the samples does not affect the magnetic transition observed and the transition is an intrinsic property of the Al-Cu-Ge-Mn host alloy.Samples of icosahedral quasicrystals were kindly provided by Profs. A. Inoue, T. Masumoto and P. H. Shingu. Ball milling was performed in Kyoto University by a courtesy of Prof. P. H. Shingu. This work was supported by the project for priority areas on properties of quasicrystals (No. 01630003) from the Japanese Ministry of Education, Science and Culture.     

Magnetic behaviour ofCuAuFe alloys

The magnetic properties of Cu_99-xAu_xFe₁ alloys (x=12, 37 and 50.7 ats) have been investigated over the temperature range 4.2–70 K using low field AC magnetic susceptibility measurements and mössbauer spectroscopy. All alloys exhibit spin glass behaviour at low temperature with freezing temperatures T_f-5.7–7.6 K. Results of analysis of the high temperature (T3 T_f) Curie-Weiss behaviour are compared with those obtained from analysis of the broadly distributed 4.2 K Mössbauer spectra.     

Mössbauer study of local environment effects in the ordered Fe70Al30 Invar alloy: Temperature dependence of isomer shift in the spin-glass phase

The systematic studies of the magnetic hyperfine field distribution for ⁵⁷Fe in the spin-glass (SG) phase of the ordered Fe₇₀Al₃₀ Invar alloy have been performed using Mössbauer spectroscopy technique in the temperature range from 5 to 80 K. Particular emphasis has been placed on the low-field component of the distribution, which is considered as corresponding to the Fe sites in the SG magnetic configurations. The main result is the observation of the pronounced temperature dependence of isomer shift for several atomic SG configurations. The temperature behavior of the local electron density is strongly correlated to the Invar properties of the Fe₇₀Al₃₀ alloy. We argue that the observed temperature dependence of the isomer shift due to a local volume effect. The temperature range, for which the pronounced decrease in atomic volume is observed, coincides with the range of the existence of the Invar effect. The influence of the competition between opposite in sign exchange interactions on the Invar properties is discussed.     

Spin glass behavior probed by various methods with different time- and space-scale of observation: Ising spin glass Fe0.50Mn0.50TiO3

Under the expectation that the behavior of a spin glass (SG) system shows various aspects depending on the time- and space-scale of observations, we have studied the typical Ising spin glass Fe_0.50Mn_0.50TiO₃ by measuring dc-magnetization, ac-susceptibility, Mössbauer spectrum, neutron scattering intensity and μ⁺SR time spectrum. We have demonstrated that the application of various methods with different time- and space-scale of observations to the same system is useful to clarify the property of the spin glass freezing, the Ising character and the de Almeida and Thouless-line.     

AC susceptibility enhancement studies in magnetic systems

Enhancement of AC susceptibility has been observed for typical ferromagnets (Gd), reentrant spin glasses like (Fe_1.5Mn_1.5Si) and canted spin systems (Ce(Fe_0.96Al_0.04)₂). The data have been interpreted with the help of a simulation model based on dry friction-like pinning of domain walls for systems having ferromagnetic domain structures. A strong pinning mechanism appears in the reentrant spin glass like and canted spin systems at low temperatures in addition to the intrinsic one in the ferromagnetic phase. The temperature variation of the pinning potential has been given qualitatively for the reentrant spin glass like systems.     

Characterization of magnetic phases in the FexMn0.65−xAl0.35 disordered alloys

Melted alloys of the Fe_xMn_0.65−xAl_0.35 disordered system, 0.25?x?0.65, were experimentally studied by Mössbauer spectrometry, vibrating sample magnetometry and AC magnetic susceptibility. All the alloys exhibit the BCC structure with a nearly constant lattice parameter (2.92 Å). Mössbauer studies at room temperature (RT) show that in the 0.25 ?x?0.45 range the alloys are paramagnetic (P) while in the 0.50?x?0.65 range, they are ferromagnetic. At 77 K, Mössbauer studies show that the alloy with x=0.25$x=0.25$ presents weak magnetic character that is consistent with an antiferromagnetic (AF) behavior due to the high Mn content, while those with 0.30?x?0.40 are paramagnetic, and those in the 0.45?x  ?0.65 range are ferromagnetic (F) with a mean field increasing with the Fe content. Hysteresis cycles at RT prove the paramagnetic character of the alloys between x=0.25$x=0.25$ and 0.40 and the ferromagnetic character for x?0.45$x?0.45$. Complementary measurements using AC magnetic susceptibility permit a magnetic phase diagram to be proposed, with the P phase for high temperature and all the compositions, the AF phase for low Fe content and at low temperature, the F phase for high Fe content above RT and the spin glass phase for all the compositions and at temperatures lower than 46 K. In addition, the mean field renormalization group (MFRG) method, applied to a random competitive and site dilute Ising model with nearest-neighbor, gives rise to magnetic phase diagram, which fairly agrees with previous experimental one.     

Mössbauer investigation of Fe0.5In1.5S3

⁵⁷Fe Mössbauer measurements are reported on a cubic spinel with nominal composition Fe_0.5In_1.5S₃ in the temperature range 4.3 K to 295 K. An occupation ratio of 0.05:1 was determined for Fe in the tetrahedral A and octahedral B positions. Below 10 K evidence for the appearance of a spin glass state is obtained.     

A57Fe Mössbauer study of Nd(Fe0.5Co0.5)9Si2

A⁵⁷Fe Mössbauer study of Nd(Fe_0.5Co_0.5)₉Si₂ has been carried out over the temperature range 4.2–295 K. The analysis of the Mössbauer spectra, combined with X-ray diffraction on a magnetically aligned powder sample, shows that the easy-magnetization direction lies in the basal plane of this tetragonal BaCd₁₁ structure at 295 K, but is canted at an angle of 29(5) above the basal plane at 4.2 K. AC susceptibility measurements performed in the temperature range 77–295 K reveal a peak spanning the range 87–106 K, with the maximum occurring at 96 K. From these data, we conclude that there is a spin-reorientation from basal c-plane to a canted magnetic structure in this compound, with an onset at 96 K as the temperature decreases.     

Test for the influence of relaxation on Mössbauer spectra of (Fe0.65Ni0.35 1−x Mn x alloys by the sharpening method

A mathematical procedure which gives an opportunity to distinguish between relaxation and static mechanisms of the Mössbauer line broadening is developed. It is based on the method of Mössbauer line sharpening developed recently and allows one to answer unambiguously the question whether or not relaxation manifests itself in Mössbauer measurements by examinign the wings of the spectrum. The procedure was applied to the spectra of (Fe_0.65Ni_0.35)_1–x Mn _x alloys withx=0 (INVAR) andx=0.047, where the mechanism of the line broadening has not been clarified so far. An analysis of the spectra shows that in the temperature range 4 to 300 K no relaxation is observed and the line broadening is mainly caused by the distributions of magnetic hyperfine fields.     

Nanowires of iron oxides embedded in SiO2 templates

To attain the complete filling of the channels of MCM-41 with magnetite and maghemite, we have tried out an alternative method to the incipient wetness impregnation. The mesoporous material was instilled with a Fe-carrying organic salt after subjecting the matrix to a silylation treatment. Thus, a solid of 7.7 wt.% iron-loaded MCM-41 was obtained. Different subsequent thermal treatments were used to produce γ-Fe₂O₃ or Fe₃O₄. The Mössbauer and magnetic results show that after this method, the as-prepared composite displays a size-distribution of magnetic particles. It is mainly made up of fine particles that display a superparamagnetic relaxation at room temperature and get blocked at ≈42 K for the AC susceptibility time-scale measurements both for γ-Fe₂O₃ and Fe₃O₄ particles. For both samples, about 24% of larger iron-containing phases are magnetically blocked at room temperature. For the Fe₃O₄ particles, this fraction undergoes the Verwey transition at about 110 K; in addition, there is a minor Fe (III) fraction that remains paramagnetic down to 4.2 K.     

57Fe high pressure Mössbauer and X-ray studies of Gd2Fe17C x interstitial compounds

The unit cell volume dependence of the Curie temperature of Gd₂Fe₁₇ is studied by means of high-pressure Mössbauer spectroscopy. From the pressure dependence of the average isomer shift of Ge₂Fe₁₇ at room temperature, the contribution of the pure magnetovolume effect to the change of the average isomer shift is derived. By combining the Mössbauer measurements of Gd₂Fe₁₇C _x with different C concentrations at room temperature, the change ofIS in Gd₂Fe₁₇C _x is dominated by the magnetovolume effect. The contribution of the chemical bonding effect is about 24% of that of the magnetovolume effect, but with negative sign.     

Mössbauer study of Lu2Fe3O7: A two-dimensional antiferromagnet on a triangular lattice

Mössbauer studies reveal that there are two kinds of Fe³⁺ spins with completely different characteristics in Lu₂Fe₃O₇: one is an Ising-like property and the other is a Heisenberg-like property in a two-dimensional antiferromagnet on a triangular lattice. The former spin orders ferrimagnetically along thec-axis at around 220 K. The latter spin is lying in thec-plane and a corresponding hyperfine magnetic field is observed at temperatures below 50 K. At very low temperatures, however, the latter spin has a component parallel to thec-axis and couples with the former spin. This finding is consistent with the modulated profile of the magnetic scattering in neutron diffraction and the result of a magnetization measurement.