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.     

The temperature dependence of the57Fe hyperfine magnetic field distribution in Fe-Ni

The temperature dependence of the⁵⁷Fe hyperfine magnetic field (hmf) in Fe-Ni is stronger than the temperature dependence of the⁵⁷Fe hmf in pure Fe. By analyzing the shape of the⁵⁷Fe hmf distribution, and with the help of experiments with Si in Fe-Ni, we deduce that this anomalous temperature dependence originates from a large thermal sensitivity of the magnetic moments at those Fe atoms with more Ni nearest neighbors. A strong temperature dependence of the recoilfree fraction was also observed in Fe-Ni alloys. We suggest that a large mean square thermal displacement of Fe atoms in Fe-Ni is the cause of the anomalous temperature dependence.     

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.     

Hyperfine Interaction Studies on Y, Zr, Nb, Mo, Rh, In and Xe in Co

Nuclear magnetic resonance on oriented nuclei and modulated adiabatic fast passage on oriented nuclei measurements were performed on several 4d and 5sp impurities in polycrystalline Co(fcc) foils and Co(hcp) single crystals. The hyperfine fields of Y and Zr in Co(fcc), the hyperfine fields of Y, Zr, Nb, Mo, Rh, In and Xe in Co(hcp), the electric field gradients of Zr, Nb and In in Co(hcp), and the nuclear spin-lattice relaxations of Zr, Nb, Rh and In in Co(hcp) were determined. The dependence of the hyperfine fields and electric field gradients in Co(hcp) on the angle between the magnetization and the c axis was investigated in most cases. The magnetic-field dependence of the spin-lattice relaxation was studied for Nb, Rh and In in Co(hcp), applying the magnetic field perpendicular to the c axis. The known hyperfine interaction parameters of the 4d and 5sp impurities in Co(fcc) and Co(hcp) are summarized. The new results provide a more detailed picture of the hyperfine interaction in Co.     

Heavy Ion Irradiated Ferromagnetic Films: The Cases of Cobalt and Iron

Polycrystalline, e-gun deposited Co, Fe and Co/Fe films, tens of nanometers thick, have been irradiated with Ne, Kr, Xe and/or Fe ions to fluences of up to 5 × 10¹⁶ ions/cm². Changes in the magnetic texture induced by the implanted ions have been measured by means of hyperfine methods, such as Magnetic Orientation Mössbauer Spectroscopy (Fe), and by Magneto-Optical Kerr Effect and Vibrating Sample Magnetometry. In Co and CoFe an hcp → fcc phase transition has been observed under the influence of Xe-ion implantation. For 10¹⁶ Xe-ions/cm², ion beam mixing in the Co/Fe system produces a soft magnetic material with uniaxial anisotropy. The effects have been correlated with changes in the microstructure as determined via X-ray diffraction. The influences of internal and external strain fields, an external magnetic field and pre-magnetization have been studied. A comprehensive understanding of the various effects and underlying physical reasons for the modifications appears to emerge from these investigations.     

Local magnetic states and hyperfine interactions in Fe/Ti magnetic superlattices

Multilayer Fe/Ti films are synthesized by deposition in a Penning discharge. Measurements are made of thhe static hysteresis loops and Mössbauer spectra on Fe⁵⁷ nuclei. The hyperfine magnetic field distribution functions are calculated. It is established that the spontaneous magnetization of Fe/Ti magnetic superlattices undergoes very strong oscillations as a function of the Ti layer thickness. Three groups of peaks are noted in the hyperfine field distribution functions, corresponding to three nonequivalent states of the Fe ions, in one of which these ions do not have a characteristic magnetic moment. These results also agree with measurements of the temperature dependence of the magnetization in weak magnetic fields. For some Ti interlayer thicknesses the saturation magnetization scaled to the Fe content is much higher than the saturation magnetization of bulk Fe.     

Noncollinear magnetic hyperfine fields in the Ag spacers of Fe/Ag multilayers

Nearly perpendicular magnetic hyperfine fields have been observed for the first time in the Ag "spacers" of Fe/Ag multilayers using low temperature nuclear orientation of (110)Ag(m) at 6 mK. At the same time, vibrating sample magnetometry measurements at temperatures down to 4 K have shown the magnetic anisotropy of the Fe to be in plane. The direction of the Ag hyperfine field is thus noncollinear (nearly orthogonal) to the Fe anisotropy. These results are compared with full potential linearized augmented plane wave calculations using the wien97 code.     

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.     

Investigations of “soft-landed” Cd surface atoms via nuclear methods: hyperfine-field sign determination

Using refined preparation techniques, cadmium guest atoms have been positioned at different sites on the surfaces of nickel crystals. The magnetic hyperfine fields and the electric field gradients at the Cd nuclei were measured by time-dependent perturbed angular correlation (TDPAC) spectroscopy of the emitted gamma radiations. By measuring the combined interactions, electric field gradients and magnetic hyperfine fields can be unambiguously attributed to each surface site. The signs of the magnetic hyperfine fields are determined by applying an external magnetic field and choosing the appropriate γ-ray detector configuration. The measured fields correlate with the number of neighbouring host atoms. Band structure calculations confirm this finding and predict magnetic fields for various sp elements from the band structure of the s-like conduction electrons. The quadrupolar interactions are manifestations of the balance in the occupation of the guest p-sublevels. These results provide new information on the structure and formation of electronic configurations of sp elements in different local environments and will contribute to understanding electronic effects on surfaces.     

Theoretical investigation of Mössbauer hyperfine interactions in ordered FeNi and disordered Fe–Ni alloys

Electronic structure spin-polarized calculations were performed for 79-atoms embedded clusters representing the ordered intermetallic compound FeNi, the fcc Fe-rich disordered alloy Fe₈₅Ni₁₅ in an antiferromagnetic (AFM) configuration, and the ferromagnetic (FM) disordered alloy Fe₅₀Ni₅₀. The spin-polarized discrete variational method (DVM) in Density Functional theory was employed. Spin magnetic moments, as well as the ⁵⁷Fe Mössbauer hyperfine parameters isomer shift and magnetic hyperfine fields, were obtained from the calculations. For FM Fe₅₀Ni₅₀, the effect of pressure on the hyperfine field and on the isomer shift was investigated, for three different local atomic configurations surrounding the ⁵⁷Fe probe atom. In the case of the isomer shift, the calculated values were compared to reported experimental data.     

Calculation of hyperfine interaction parameters in metals-friedel oscillations in dilute Fe and Cu alloys

We review some recent calculations on hyperfine interaction parameters in metals based on density functional theory in the local density approximation. We restrict ourselves to the calculation of Friedel oscillations of the charge and magnetization density in dilute Fe and Cu alloys. In particular, we estimate hyperfine fields, isomer shifts and electric field gradients for a few shells around the impurities. The calculations are performed using the KKR-Green's function method. Especially, we discuss which valence properties determine the hyperfine interaction parameters and what information about the electronic structure can be obtained from their measurement.     

Role of the chemical ordering on the magnetic properties of Fe–Ni cluster alloys

The spin and orbital moments of fcc Fe-Ni cluster alloys are determined within the framework of a d-band Hamiltonian including the spin-orbit coupling non perturbatively. Different sizes (up to 321 atoms), compositions, and chemical configurations (random alloys as well as core-shell arrays of iron and nickel atoms) are considered in order to reveal the crucial role played by local order and stoichiometry on the magnetic moments of the clusters. Interestingly, we have found considerably reduced average magnetizations for Fe-Ni clusters with Fe cores compared to that of the bulk alloy with the same composition. Indeed, in these configurations not only antiparallel arrangements between the local moments of some Fe atoms within the iron core are found, but also the total magnetization of the surface Ni atoms is significantly quenched. On the opposite, the disordered and Ni-core cluster alloys are characterized by high magnetizations resulting from saturated-like contributions from both Ni and Fe atoms, in agreement with recent ab-initio calculations. In general, the local orbital magnetic moments are strongly enhanced with respect to their bulk values. Finally, the variation of the orbital-to-spin moment ratio with the chemical order is discussed.     

Mössbauer effect in natural strunzite, ferristrunzite and ferrostrunzite

The temperature dependence of the ferric and ferrous hyperfine fields in natural samples of strunzite, ferristrunzite and ferrostrunzite is determined by Mössbauer spectroscopy between 4.2 K and their magnetic transition temperatures (T _N), i.e. 50.5±0.5 K, 43.0±0.5 K and 44.0±0.5 K respectively, which are determined by Mössbauer thermoscanning. Two dominating magnetically split ferric subspectra were consistently present in all of the samples and are related to the Fe(1) and Fe(2) sites in the crystallographic structure, but an unambiguously assignment to a specific site is not possible. The difference between the corresponding hyperfine fields is very small. In the strunzite sample these fields are well defined and rather weakly dependent of temperature. In the other samples the corresponding hyperfine fields are more distributed especially at higher temperatures (below T _N). The relative contribution in the spectra of the third magnetic ferric component differs strongly between the samples and is assigned to ferric ions at the Mn site. At the lowest temperatures applied, its hyperfine field exceeds all other field values, but it decreases rather rapidly with increasing temperature, in so far that the corresponding spectral lines make a crossover with the lines of the other ferric subspectra. The magnetically split spectra of ferrostrunzite consist additionally of a ferrous magnetic component, which could be successfully analysed by introducing two magnetically split ferrous subspectra, which strongly overlap with each other but also with the ferric components. At higher temperatures in the magnetic region all subspectra overlap more and in the case of ferri- and ferrostrunzite the ferric hyperfine fields were distributed over a wider range.     

Electronic structure of Ru impurities in iron

The molecular cluster discrete variational method has been employed to study the magnetic properties of Ru impurities and Ru monolayers in iron. With the introduction of Ru atoms in the neighborhood of an Fe atom the local moment changes appreciably and the magnetization decreases steadily. By increasing Ru concentration both ferromagnetic and antiferromagnetic Fe–Ru couplings can be expected in dilute alloys. The calculations indicate that the contact hyperfine fields of Fe atoms are strongly dependent on the chemical environment as well as on the local symmetry.     

Iron oxidation, interfacial expansion, and buckling at the Fe/NiO(001) interface

In order to provide a structural basis for a physical understanding of exchange bias in metal/magnetic-oxide interfaces, we have determined the structure of the Fe/NiO(001) interface by means of x-ray absorption spectroscopy and ab initio density functional theory calculations. A Fe-Ni alloyed phase on top of an interfacial FeO planar layer is formed. The FeO layer exhibits a 7% expanded interlayer distance and a 0.3 A buckling; its presence is predicted to increase the spin magnetic moment of the interface Fe atoms by 0.6 mu(B), compared to the ideally abrupt interface.     

Magnetic moments and hyperfine fields at Fe in 3d-transition metals

The magnetic moments and hyperfine fields at Fe sites in 3d-transition metals are calculated using the first principle discrete variational method in local density approximation. Although a large positive moment is retained at each Fe site, the hyperfine fields varied from large negative to large positive values. It is concluded that the absence of Mössbauer magnetic splitting does not necessarily imply the absence of local magnetic moments.     

Spin-canting and transverse relaxation in maghemite nanoparticles and in tin-doped maghemite

The magnetic properties of maghemite nanoparticles and tin-doped maghemite have been studied by ⁵⁷Fe and ¹¹⁹Sn Mössbauer spectroscopy at temperatures from 6 to 300 K with and without applied magnetic fields. The low-temperature ⁵⁷Fe spectra of both samples, obtained in a field of 4 T, can be described in terms of A-site and B-site components with perfect ferrimagnetic order and a strongly canted component, which seems to have its main contribution from B-site ions. At higher temperatures, the components with strong canting are influenced by transverse relaxation, which results in significant line broadening, a reduction of the magnetic hyperfine splitting and a reduction in the relative areas of lines 2 and 5. The ¹¹⁹Sn spectra show a very broad distribution of magnetic hyperfine fields at low temperatures. When the sample was exposed to applied magnetic fields the distribution became narrower. The spectra show that the direction of the hyperfine field of a large fraction of the tin ions in maghemite is antiparallel to the applied field, but a minor fraction of the tin ions have canted hyperfine fields.     

Hyperfine interactions and electronic structures of BaFe 2 As 2 : a first-principles LDA+U study

The hyperfine parameters of hyperfine fields, electric field gradients and isomer shifts at the Fe site are investigated based on the first-principles calculations of the electronic structures using LDA (GGA)+U method in the low-temperature orthorhombic antiferromagnetic phase of undoped BaFe₂As₂. It is fond that the electric field gradient of Fe nucleus is highly related with the electronic structures close to the Fermi level. Though the addition of negative on-site Coulomb interaction to Fe-3d states improves the calculated magnetic moment of Fe atom and the hyperfine parameters of Fe nucleus when U = ?0.1 Ry (?0.08 Ry) for GGA+U (LDA+U) method, a negative U correction does not capture the right physics of this system. The calculations prove the strong coupling between the magnetic, structural and electronic properties in antiferromagnetic BaFe₂As₂ parent.     

Invar Behavior in Fe-Ni Alloys is Predominantly a Local Moment Effect Arising from the Magnetic Exchange Interactions Between High Moments

I argue that the main models that have been advanced to explain Invar behavior in Fe-Ni alloys (the original, classical, Invar system) can all be shown to be critically deficient, except one: The local moment frustration model of Rancourt and Dang ( Phys. Rev. B , 54 , 12225, 1996). The latter model explains all the measured structural, magnetic, and magnetovolume features of the Fe-Ni alloys with 0-65 apc (atomic percent) Fe, based on the assumptions that these systems are predominantly high-moment in character at the temperatures of interest and that the Fe-Fe pairs have large inter-atomic separation dependencies of their magnetic exchange parameters. The large magnetovolume Fe-Fe couplings are understood (based on ab initio electronic structure calculations) as a precursor effect of the low-moment/high-moment (LM/HM) transition that has recently been observed to occur at larger Fe concentrations, as a continuous transition occurring in the range , 65-75 apc Fe (Lagarec, Ph.D. thesis, 2001).     

On the origin of discontinuity of the hyperfine fields at Fe nuclei in bulk iron and aerosol Fe nanoparticles

Advancing the early work in which a discontinuity of hyperfine fields at ⁵⁷Fe nuclei in bulk iron and in aerosol Fe nanoparticles has been revealed by analyzing their Mössbauer spectra the present Letter evidences that the existence of several peaks in the hyperfine distribution (HFD) for bulk Fe is caused with the internal magnetic fields owing to its multidomain structure whereas aerosol Fe nanoparticles are single-domain and show only a unique peak in HFD. This argument has been corroborated by transformation of the HFD pattern for Fe foil after applying the external magnetic field of 0.03 T.