Large orbital moments and internal magnetic fields in lithium nitridoferrate(I)

The iron nitridometalates Li2[(Li(1-x)Fe(I)(x))N] display ferromagnetic ordering and spin freezing. Large magnetic moments up to 5.0mu(B)/Fe are found in the magnetization. In M?ssbauer effect studies huge hyperfine magnetic fields up to 696 kOe are observed at specific Fe sites. These extraordinary fields and moments originate in an unusual ligand field splitting for those Fe species leading [within local spin density approximation (LSDA)] to a localized orbitally degenerate doublet. Including spin-orbit interaction and strong intra-atomic electron correlation (LDA+SO+U) gives rise to a large orbital momentum.     

A Mössbauer effect study of Y(57Fe:Mn)12

The intermetallic compound, YMn₁₂, doped with 0.5at.%⁵⁷Fe has been investigated using the⁵⁷Fe Mössbauer resonance. The data show that the Fe impurities occupy preferentially the f-site at the expense of the i- and j-sites. Whereas the i- and j-sites are expected to carry identical local magnetic moments in the ordered state, low temperature hyperfine fields of 50.08(±0.05)T and 2.90(±0.03)T are measured for the i- and j-sites respectively. It is proposed that large transferred hyperfine fields are responsible for this disparity.     

Application of M?ssbauer spectroscopy in magnetism

An overview is provided on our recent work that applies ⁵⁷Fe M?ssbauer spectroscopy to specific problems in nanomagnetism. ⁵⁷Fe conversion electron M?ssbauer spectroscopy (CEMS) in conjunction with the ⁵⁷Fe probe layer technique as well as ⁵⁷Fe nuclear resonant scattering (NRS) were employed for the study of various nanoscale layered systems: (i) metastable fct-Fe; a strongly enhanced hyperfine magnetic field B_hf of ～39?T at 25?K was observed in ultrahigh vacuum (UHV) on uncoated three-monolayers thick epitaxial face-centered tetragonal (fct) ⁵⁷Fe(110) ultrathin films grown by molecular-beam epitaxy (MBE) on vicinal Pd(110) substrates; this indicates the presence of enhanced Fe local moments, μ_Fe, as predicted theoretically; (ii) Fe spin structure; by applying magnetic fields, the Fe spin structure during magnetization reversal in layered (Sm–Co)/Fe exchange spring magnets and in exchange-biased Fe/MnF₂ bilayers was proven to be non-collinear and depth-dependent; (iii) ferromagnet/semiconductor interfaces for electrical spin injection; CEMS was used as a diagnostic tool for the investigation of magnetism at the buried interface of Fe electrical contacts on the clean surface of GaAs(001) and GaAs(001)-based spin light-emitting diodes (spin LED) with in-plane or out-of-plane Fe spin orientation; the measured rather large average hyperfine field of ～27?T at 295?K and the distribution of hyperfine magnetic fields, P(B_hf), provide evidence for the absence of magnetically “dead” layers and the existence of relatively large Fe moments (μ_Fe ～ 1.8?μ_B) at the ferromagnet/semiconductor interface. - Finally, a short outlook is given for potential applications of M?ssbauer spectroscopy on topical subjects of nanomagnetism/spintronics.     

Local magnetic moments and hyperfine magnetic fields in Fe-M (M = Si, Sn) alloys at small metalloid concentrations

The main tendencies in the formation of local magnetic moments and hyperfine magnetic fields at Fe nuclei in Fe-Sn and Fe-Si alloys at low metalloid concentrations are analyzed on the basis of “first-principles” calculations. The results of calculations are compared with experimental data. The main differences between these alloys were proved to be due to the differences in their lattice parameters. It is shown that a significant contribution to the formation of the hyperfine field comes from the orbital magnetic moment and the Ruderman-Kittel-Kasuya-Yosida polarization, which depend on the impurity concentration and the distance to an impurity atom in the crystal lattice.     

Surface and interface studies with ASPIC

Magnetic properties at surfaces and interfaces have been investigated performing Perturbed Angular Correlation (PAC) measurements in the UHV chamber ASPIC (Apparatus for Surface Physics and Interfaces at CERN) using different PAC probes. The results are: (i) determination of magnetic hyperfine fields of Se on Fe, Co, Ni which are explained by a theoretical study on the magnetic hyperfine fields of 4sp-elements in adatom position on Ni and Fe;(ii) static magnetic hyperfine fields in ultrathin Pd on Ni(0 0 1) which indicate an induced magnetic order in Pd;(iii) the observation of induced fluctuating magnetic interactions in Pd when thick Pd is in contact with Ni. Monolayer-resolved measurements of the magnetic hyperfine fields in magnetized Pd are in accordance with theoretical predictions of the layer dependence of the induced magnetic moments in Pd. This revised version was published online in July 2006 with corrections to the Cover Date.     

A study of the magnetic moments and Fe site hyperfine fields in iron-chromium alloys

The magnetization of Fe-Cr alloys ranging from 1 to 15 atomic % of Cr has been measured at room temperature in order to study the relationship between the Fe site hyperfine fields and the magnetic moment. The average moment decreases linearly, at a rate of -2.36 μ_B per Cr atom, up to 10% Cr concentration. The Fe site hyperfine fields were measured in a previous study¹ using the same samples. It is found that the hyperfine fields measured are not proportional to the corresponding magnetic moments. The results are interpreted using a model previously developed for other binary alloys of iron².     

Absence of magnetism in hcp iron-nickel at 11 K

Synchrotron M?ssbauer spectroscopy (SMS) was performed on an hcp-phase alloy of composition Fe92Ni8 at a pressure of 21 GPa and a temperature of 11 K. Density functional theoretical calculations predict antiferromagnetism in both hcp Fe and hcp Fe-Ni. For hcp Fe, these calculations predict no hyperfine magnetic field, consistent with previous experiments. For hcp Fe-Ni, however, substantial hyperfine magnetic fields are predicted, but these were not observed in the SMS spectra. Two possible explanations are suggested. First, small but significant errors in the generalized gradient approximation density functional may lead to an erroneous prediction of magnetic order or of erroneous hyperfine magnetic fields in antiferromagnetic hcp Fe-Ni. Alternately, quantum fluctuations with periods much shorter than the lifetime of the nuclear excited state would prohibit the detection of moments by SMS.     

Magnetic properties, Mössbauer effect and first principle calculations study of laves phase HfFe2

The magnetic properties and hyperfine interaction parameters for Laves phase HfFe₂ with C14 type structure are studied using SQUID magnetometer and M?ssbauer measurement. The saturation magnetization, remanent magnetization, coercive field, magnetic moment per unit formula and the hyperfine magnetic field at Fe site are reported. In addition, a detailed theoretical study of the electronic structure and hyperfine magnetic fields of the two possible HfFe₂ structures, C15 and C14, is presented. Using the full-potential linearized augmented plane wave (FP-LAPW) method as implemented in the WIEN 97 package, the equilibrium volume, bulk moduli, magnetic moments and hyperfine magnetic fields for the two structures are calculated. The obtained results are compared with the measured data.     

Effect of vanadium neighbors on the hyperfine properties of iron–vanadium alloys

The electronic and magnetic structures of Fe–V alloys are calculated using the discrete-variational and full-potential linearized-augmented-plane wave methods. The derived hyperfine properties at Fe sites are studied against the number of Fe atoms in the neighbouring shells. As expected the magnetic hyperfine field depends strongly on the number of Fe atoms in the first and second shells of neighbours while its dependence on the variation of atoms in the third shell is weak. The calculated distribution of the magnetic hyperfine fields at the Fe sites, are compared to the experimental data of Krause et al. (Phys Rev B 61:6196–6204, 2000). The contact charge densities and the magnetic moments are also calculated. It was found that the contact charge density increases with increasing V contents and this leads to negative isomer shift on addition of V.     

Local magnetic ordering of Fe impurities in Pd2MnSn

Mössbauer effect of Fe⁵⁷ embedded as very dilute substitutional impurities in Pd₂MnSn was studied. The impurities are seen to replace the three elements in the alloy. Although the Curie temperature of the alloy is 189K, well below the room temperature, the Mössbauer spectrum recorded at room temperature consisted of two distinct 6-finger magnetic hyperfine spectra and a single unsplit line. One of the 6-finger patterns which corresponds to an internal magnetic field ofH _int=?375 kOe is inferred to arise due to local magnetic coupling of the localized magnetic moments of Fe impurities at the Pd sites with those of the 4 Mn first nearest neighbours of the Fe impurities. The other 6-finger pattern which corresponds to an internal magnetic field ofH _int=?335 kOe is inferred to arise due to the local magnetic coupling of the localized magnetic moments of the Fe impurities at the Sn sites with those of the 6 Mn second nearest neighboours of the Fe impurities. The difference in the internal magnetic fields observed at the Pd and Sn sites in the alloy could be understood qualitatively, on the basis of RKKY theory, as arising due to the different conduction electron polarization contributions to the net internal magnetic field at the Fe impurity sites. The results of the measurements suggest that the localized magnetic moments of Fe⁵⁷ impurities at Pd and Sn sites are antiferromagnetically coupled with the moments of their neighbouring Mn atoms.     

Magnetic properties of Fe/Nd artificial superstructure films

Multilayered films with artificial superstructures were prepared by alternately depositing Fe and Nd in ultrahigh vacuum. The magnetic properties are studied from⁵⁷Fe Mössbauer spectroscopy. The hyperfine field in Fe layers and the direction of Fe magnetic moments depend on the Fe and Nd layer thicknesses. For films with certain Fe and Nd layer thicknesses, the direction of Fe magnetic moments is in-plane at 300 K but changes to be perpendicular at low temperatures. The direction of Fe magnetic moments is discussed in relation with the magnetization of interface Nd atoms.     

First-principles studies of the magnetic hyperfine field in Fe multilayers

A detailed theoretical study of the magnetic moments and magnetic hyperfine fields in several Fe multilayers (Fe fcc(001)/5X fcc(001), X=Cu and Ag, and Fe bcc(001)/5X fcc(001), X=Ag and Au) as well as in bulk Fe is presented. The calculations have been performed using the spin-polarized, relativistic linear muffin-tin orbital (SPR-LMTO) method of band structure calculation. Therefore, not only the contribution to the hyperfine fields due to the conventional Fermi contact interaction but also due to the spin dipolar and orbital contributions induced by the crystal field and by spin-orbit coupling are accounted for. To decompose the hyperfine field of non-s-electrons into these contributions it has been assumed that they are proportional to the corresponding so-called magnetic dipole moment and the orbital magnetic moment, respectively. In contrast to previous results for pure metals and alloys not only the orbital but also the spin dipolar hyperfine field was found to be non-negligible. The anisotropy of the hyperfine field determined by calculations for in-plane and perpendicular orientation of the magnetisation was found to be very pronounced and closely connected with the corresponding anisotropy of the magnetic dipole moment and the orbital moment.     

Hyperfine magnetic fields in Fe−Co alloys and their tempera ture dependences

We obtained⁵⁷Fe hyperfine field parameters from Fe₁−x-Co _x alloys (0≤x≤0.6) from 77 K to 900 K. We first discuss the origin of the low temperature hyperfine fields in terms of the 3d and 4s electrons at⁵⁷Fe atoms. The⁵⁷Fe hyperfine magnetic field (hmf) of Fe-Co alloys depends more weakly on temperature than the hmf of pure Fe. This temperature dependence occurs because the alignment of the magnetic moments at both the Fe atoms and at the Co atoms depend on temperature in the same way as the bulk magnetization of Fe-Co alloys.     

Conversion electron Mössbauer spectroscopic study of YIG substituted with Bi,Ti, Ga and La

YIG films, substituted with Bi, Ti, Ga and La, were grown on a (111) plane of Gd₃Ga₅O₁₂ or (Gd, Ca)₃(Ga, Mg, Zr)₅O₁₂ by a liquid phase epitaxial method. With the increase of the concentration of Bi atoms, which are substituted at 24c sites of YIG, the magnetic hyperfine fields at 16a and 24d Fe sites increased and the direction of magnetic moments changed from parallel to 45° to the (111) plane. With the increase of Ga concentration, the hyperfine fields at 16a and 24d Fe sites decreased. The hyperfine interaction and the substitution effect of YIG films are discussed.     

A fully relativistic description of the hyperfine interaction in magnetic systems

Based on the spin-polarized version of the multiple scattering theory, a relativistically correct formulation for the Green’s function describing the electronic structure of magnetic metallic systems has been derived. By this way, orbital contributions to the magnetic moment and, for the first time, to the hyperfine fields, which are caused by an unquenching of the orbital momentum due to spin-orbit coupling, were accessible to a calculation. In the case of Fe, Co and Ni, it has been found, that the corresponding non-s-contributions to the hyperfine field of the conduction electrons stem nearly exclusively from the d-electrons, are positive and of the same order of magnitude as the s-part of the conduction band contribution to the total hyperfine field. In all three cases these large non-s-hyperfine fields compensate the relativistic enhancement of the (Fermi contact) s-hyperfine field compared to a non-relativistic calculation, leading to theoretical hyperfine fields which are below the experimental ones. At the moment, it cannot be decided whether this discrepancy is caused by the neglect of the non-s-contributions of the core electrons or shortcomings of the local spin density approximation.     

Magnetism of linear chains

Accurate self-consistent local spin density electronic structure calculations for linear chains of Ni and Fe atoms are presented which realistically treat three-dimensional nature. The one-dimensional character of the bands manifests itself in high density of states arising from van Hove singularities. Both transition metals are “strong” Stoner ferromagnets with large magnetic moments (3.3 and 1.1μ_B for Fe and Ni, respectively) and have large s- and d-exchange splittings. From fits of our results to simple tight-binding models, we find that the d-d effective exchange interaction is similar to that in bulk. However, the use of standard bulk tight-binding parameters is found to be inappropriate since they qualitatively change the results by, for example, misplacing the Fermi level with respect to the band edges. Moreover, in contrast to the bulk, the linear chains also show a rather large s-exchange interaction and hence a large and positive valence contribution to the contract hyperfine field; for Fe this results in a positive contact hyperfine field of the same magnitude as in the bulk. The unique signatures of these linear systems should make their characterization experimentally feasible.     

First-principles calculations for alloyed cementite (Fe–Ni)<Subscript>3</Subscript>C

First-principles calculations for the electron structure of cementite doped with Ni are performed. The obtained data for magnetization, local magnetic moments, and parameters of hyperfine interaction at Fe nuclei are compared with those for pure cementite and used to interpret experimental magnetic and Mössbauer data for the alloyed cementite obtained through mechanical alloying with Ni.     

Hyperfine interactions in Sc<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Y<Subscript>x</Subscript>Fe<Subscript>2</Subscript> cubic Laves alloys

Effects of hybridization of 3d bands of iron with 3d bands of scandium and 4d bands of yttrium in Sc_1?xY_xFe₂ cubic Laves alloys (0≤_x≤1) are studied by the nuclear magnetic resonance method. The concentration dependences of the lattice parameters a, saturation magnetization σ, and hyperfine fields at the ⁵⁷Fe, ⁴⁵Sc, and ⁸⁹Y nuclei—as well as the ²⁷Al impurity nuclei, whose atoms substitute iron atoms in the lattices of these alloys—are measured. The “local” and “induced” contributions to hyperfine fields at the ⁵⁷Fe nuclei are separated and the magnetic moments at iron atoms are estimated. It is found that the hybridization effect leads to the formation of magnetic moments at Sc and Y atoms (whose direction is opposite to the direction of the magnetic moment at iron atoms) and is responsible for the ferrimagnetic structure in Sc_1?xY_xFe₂ alloys.     

Magnetism of Fe in SrFe2As2: Local investigation by time differential perturbed angular distribution (TDPAD) spectroscopy

Employing the γ-ray perturbed angular distribution technique, we have measured the magnetic hyperfine field of ⁵⁴Fe in tetragonal and orthorhombic structural phases of SrFe₂As₂. In the tetragonal phase, the magnetic response of ⁵⁴Fe shows Curie-Weiss type local susceptibility, indicating the presence of localized moment on Fe. The temperature dependence of the hyperfine field of ⁵⁴Fe reflects quasi-two dimensional first order magnetic transition at 200 K. Our data indicate that Fe moments in the magnetically ordered phase of SrFe₂As₂ may be canted out of the ab-plane.     

The Electronic and Magnetic Properties of FCC Iron Clusters in FCC 4D Metals

The electronic and magnetic structures of small FCC iron clusters in FCC Rh, Pd and Ag were calculated using the discrete variational method as a function of cluster size and lattice relaxation. It was found that unrelaxed iron clusters, remain ferromagnetic as the cluster sizes increase, while for relaxed clusters antiferromagnetism develops as the size increases depending on the host metal. For iron in Rh the magnetic structure changes from ferromagnetic to antiferromagnetic for clusters as small as 13 Fe atoms, whereas for Fe in Ag antiferromagnetism is exhibited for clusters of 24 Fe atoms. On the hand, for Fe in Pd the transition from ferromagnetism to antiferromagnetism occurs for clusters as large as 42 Fe atoms. The difference in the magnetic trends of these Fe clusters is related to the electronic properties of the underlying metallic matrix. The local d densities of states, the magnetic moments and hyperfine parameters are calculated in the ferromagnetic and the antiferromagnetic regions. In addition, the average local moment in iron-palladium alloys is calculated and compared to experimental results.