Magnetic surface anisotropy of transition metal ultrathin films

In order to study the magnetic anisotropy of transition metal ultrathin films, we have performed tight-binding calculations including spin-orbit coupling. Beside the anisotropy energy these calculations also yield the orbital moment, which turns out to be much more anisotropic than in bulk materials. The effects of interfacial mismatch and roughness are discussed within phenomenological models. We also briefly review experimental results on the magnetic surface anisotropy (MSA) in transition metal ultrathin films. In some cases such as Au/Co/Au(111) sandwiches the MSA wins the competition with the shape anisotropy arising from the magnetostatic energy: below a critical thickness this leads to aperpendicular spontaneous magnetization. We show the effects of this crossover on the hysteresis loops and on the magnetoresistance, and the effects of interface roughness on the critical thickness.     

Surface electronic structure of Gd(0001) films on W(110)

Received: 1 September 1996/Accepted: 6 January 1997     

Ferromagnetism in the thermodynamically stable monolayer Fe(110) on W(110), coated by Ag

Ferromagnetic order in the thermodynamically stable, pseudomorphic monolayer Fe(110) on W(110), coated by Ag, was studied in situ in UHV using Conversion Electron Mössbauer Spectroscopy (CEMS) and Torsion Oscillation Magnetometry (TOM). Films near the monolayer coverage, prepared at 475 K, consist of nearly independent monolayer and double-layer patches. The properties of monolayer patches are nearly independent of the mean film thickness resulting in excellent conditions to determine the true monolayer properties. The Curie temperature is reduced toT _{c, mono}= 282 K = 0.27 T_c,bulk, the ground state hyperfine field is reduced toB _hf(0)=11.9 T = 0.35B _hf,bulk(0) and the magnetic moment per atom is enhanced to(0) = 2.53 _B=1.14(0)_bulk. Remanent magnetization is detected forT 260 K=0.92T _{c, mono}, square loop magnetization forT 230 K=0.82T _{c, mono}. Unusual properties of the phase transition are detected by the combination of both experimental techniques.     

Development of magnetic anisotropies in ultrathin epitaxial films of Fe(001) and Ni(001)

Ultrathin films, bcc Fe(001) on Ag(001), fcc Fe(001) on Cu(001) and Fe/Ni(001) bilayers on Ag, were grown by molecular beam epitaxy. A wide range of surface science tools were employed to establish the quality of epitaxial growth. Ferromagnetic resonance and Brillouin light scattering were used to extract the magnetic properties. Emphasis was placed on the study of magnetic anisotropies. Large uniaxial anisotropies with easy axis perpendicular to the film surface were observed in all ultrathin structures studied. These anisotropies were particularly strong in fcc Fe and bcc Fe films. In sufficiently thin samples the saturation magnetization was oriented perpendicularly to the film surface in the absence of an applied field. It has been demonstrated that in bcc Fe films the uniaxial perpendicular anisotropy originates at the film interfaces. In situ measurements indentified the strength of the uniaxial perpendicular anisotropy constant at the Fe/vacuum, Fe/Ag and Fe/Au interfaces asK _us = 0.96, 0.63, and 0.3 ergs/cm² respectively. The surface anisotropies deduced for [bulk Fe/noble metal] interfaces are in good agreement with the values obtained from ultrathin films. Hence the perpendicular surface ansiotropies originate in the broken symmetry at abrupt interfaces. An observed decrease in the cubic anisotropy in bcc Fe ultrathin films has been explained by the presence of a weak 4th order in-plane surface anisotropy,K _1S=0.012 ergs/cm². Fe/Ni bilayers were also investigated. Ni grew in the pure bcc structure for the first 3–6 ML and then transformed to a new structure which exhibited unique magnetic properties. Transformed ultrathin bilayers possessed large inplane 4th order anisotropies far surpassing those observed in bulk Fe and Ni. The large 4th order anisotropies originate in crystallographic defects formed during the Ni lattice transformation.     

Magnetic dipolar interaction in ultrathin films: Structural and size effects

A previously introduced formalism for calculating magnetic dipolar anisotropy energy ΔU in atomic layered structures is further developed. Numerical results are presented for ultrathin films with different close-packed (face centered cubic (FCC) [1 1 1]) and non-close-packed (FCC [0 0 1] and body centered cubic (BCC) [0 0 1]) structures. Structural effects become apparent in the magnetocrystalline dipolar anisotropy energy ΔU_L when the ratio between the interlayer separation c and the 2D lattice constant a is changed. Despite the long-range character of the dipolar interaction, it is shown that the number of significantly interacting layers, conventially called coupled layers, is limited and depends on the structural aspect ratio c/a. The slope in the observed linear dependence between ΔU_L and the inverse of the film thickness t is explained by the number of the so-called coupled layers, and not by a surface contribution to volume values. Size effects appearing in ΔU are unambiguously distinguished from structural effects. Effective anisotropy energy ΔU_eff and ΔU are presented for Co [0 0 0 1] and Ni [0 0 1] ultrathin films. It is verified that the dipolar interaction makes an important contribution to ΔU_eff, but the spin reorientation transition is determined by non-dipolar interactions. The former favors the magnetization switching only when the size aspect ratio d/t, with d the characteristic lateral dimension of the film, is sufficiently small. Applications to other layered arrays of magnetic dipoles are straightforward.     

Magnetic hyperfine fields in ultrathin Ni films on Cu(100)

The magnetic hyperfine field was measured at ¹¹¹In(¹¹¹Cd) probe atoms in ultrathin Ni films epitaxially grown on Cu(100) utilizing the perturbed -angular correlation (PAC) method. The behaviour of the hyperfine field as a function of temperature was studied for different film thicknesses ranging from 2 up to 10 monolayers. It was found that the strength of the hyperfine fields as well as the critical temperatures are strongly reduced for thin nickel films and approach the bulk value with increasing film thickness. The orientation of the hyperfine field is discussed.     

Thickness dependence of the spin- and angle-resolved photoemission of ultrathin,epitaxial Ni(111)/W(110) layers

The thickness dependence of the magnetic band structure of ultrathin, epitaxial Ni(111)/W(110) layers has been studied by spin and angle-resolved photoemission spectroscopy. The changes of the spin-resolved photoemission intensities upon reducing the layer thickness depend strongly on the wavevector along the -L line of the Brillouin zone. The measured exchange splitting atk 1/3(-L) andk 1/2(-L) is found to be independent of the layer thickness for layers consisting of 3 or more atomic layers, while decreases rapidly with the layer thickness atk2/3(-L). This behavior is very similar to the temperature dependence of the spin-resolved photoemission spectra of bulk Ni(111) at the samek-points.     

Ferromagnetic order and critical behavior at surfaces of ultrathin epitaxial films

The critical behavior, ferromagnetic order and magnetic anisotropies of ultrathin, epitaxial, magnetic films is studied using electron capture spectroscopy (ECS), which is capable of probing the long-ranged and short-ranged electron spin polarization (ESP) at the topmost surface layer of uncoated and coated magnetic structures. For all systems [Ni(100)/Cu(100), Ni(100)/NaCl(100), fcc Fe(111)/Cu(111), Fe(100)/Ag(100), Tb/Fe(100)/Ag(100), Fe(100)/Au(100), hcp Tb(0001)/W(110), Fe(110)/W(110), V(100)/Ag(100), Pd(100)/Ag(100), Pd/W(110)] investigated so far, ferromagnetic order is detected. It is found that the surface Curie temperatureT _Cs depends on film thicknessd. ECS data obtained at the surface of various systems reveal the existence ofT- andd-dependent magnetic anisotropies. Although for V(100)/Ag(100) the measured critical exponent=0.128 agrees very well with=1/8 predicted for the two-dimensional Ising model, for other systems, such as Fe(100)/Au(100), the measured value (0.25) is in disagreement with theoretical predictions. The experimental results are discussed within the framework of presently available experimental and theoretical data.     

Depth-selective57Fe mössbauer spectroscopy: An alternative

A method to obtain depth-selective⁵⁷Fe Mössbauer spectra is described. The depth selectivity is implemented by removing thin layers from a sample and measuring the conversion-electron Mössbauer spectrum. The layer spectra, i.e. the Mössbauer spectra associated with the removed layers, are then determined by calculating the number of electrons which originate from each layer and reach the surface of the sample. The computations are based on Liljequist's theory for⁵⁷Fe conversion-electron Mössbauer spectroscopy. In this way no energy-discriminating electron spectrometers are involved, and a simple proportional counter will suffice. The depth resolution is about 20–30 nm. The method is illustrated for an ion-implanted substituted YIG film, in which case the magnetization as a function of depth is obtained.     

Magnetism in very thin films of permalloy measured by spin polarized cascade electrons

The spin polarizationP of the low energy cascade electrons excited with a primary unpolarized electron beam is measured with ultrathin films of permalloy (Ni₈₀Fe₂₀) as a function of film thickness, external magnetic field, and temperatureT. Surface adsorbates of small concentrations of less than 10% of a monolayer can change the Curie point and the saturation value ofP ₀(T0) by as much as 30%. The Ta-substrate induces a magnetically dead region in permalloy. Conventional spin wave theory cannot account for the observed smallT-dependence of the magnetizationM. Films on a nonmagnetic substrate are compared to similar films coupled to bulk permalloy over an interface of Ta. TheT-dependence ofM with the coupled films can be explained by spin wave theory. At lowT, the films coupled to the bulk exhibit a faster decrease ofM than the uncoupled films. We propose that this thermal stabilization of the magnetization in very thin ferromagnetic films is due to quenching of the long wavelength spin modes.     

In-plane magnetic surface anisotropies in Fe(110)

In-plane magnetic surface anisotropies have been detected for Fe(110) on W(110) using in situ Conversion Electron Mössbauer Spectroscopy (CEMS). The phenomenon used for the determination of this anisotropy was a switching of the spontaneous magnetizationJ _s from [001] to [1¯10] with decreasing thickness. Analysis of the data is performed using a homogeneous magnetization approximation for competing surface and bulk anisotropies, which is justified by a micromagnetic analysis and established experimentally by CEMS. In-plane surface anisotropy constants for the clean Fe(110) surface, the Fe metal-interface and the FeGaAs interface are determined toK _s,p ^FeUHV =0.065 erg·cm^–2,K _s,p ^FeMetal =0.040 erg ·cm^–2, andK _s,p ^FeGaAs =0.047 erg ·cm^–2, all with an estimated accuracy of the order of 10%.     

Large vertical loop shifts in mechanically synthesized (Mn,Fe)2O3−t nanograins

Magnetic properties of zero field cooled (ZFC) and field cooled (FC) sample of (Mn,Fe)₂O_3−t nanograins have been investigated by magnetometry (up to 70 kOe) and Mössbauer spectroscopy (up to 60 kOe) in the temperature interval 4.2–300 K. Large horizontal (up to 0.8 kOe) and vertical (up to 80%) shifts of the magnetization hysteresis loops are observed in the FC regime. The obtained results are discussed in terms of exchange interaction between an antiferromagnetic core and a spin-glass-like state of the nanograins boundaries. It is shown that hysteresis loop shifts (horizontal and vertical) depend on the field cooling magnitude, an effect that can be understood by the change of the boundary magnetic structure induced by the external magnetic field. The vertical magnetization shift is described by a phenomenological model, which takes into account the magnetic interaction between the spin-glass like boundary spins and the applied field.     

MOCVD growth, structure and magnetic properties of Fe films grown on GaAs (001) substrates

Thin iron films have been grown on (001) GaAs substrates by low pressure metal organic chemical vapor deposition (LP-MOCVD) at different temperatures with the pressure of 150 Torr. X-ray diffraction (XRD) analysis showed that all films have only one strong diffraction peak (110). The surface of Fe film became smooth with increasing the growth temperature. Magnetization measurements showed that the Fe films grown at different temperatures were ferromagnetic with easy axis parallel to the film surface and hard axis perpendicular to the substrates. The field dependence of magnetization along two axes showed a remarkable difference, implying that the samples have strong magnetic anisotropy. Furthermore, when the applied magnetic field is perpendicular to the Fe surface, a sharp jump in the hysteresis loop could be observed, followed by a broad shoulder, which is related to the interface effect, the existence of carbon and the formation of 180^°/90^° magnetic domains.     

Two-jump magnetic switching in ultrathin Co(0 0 1) films probed by giant magnetoresistance measurements

Ultrathin epitaxial FCC-Co films, which form part of a spin-valve structure, were found to undergo one- or two-jump magnetic switching, in GMR and MOKE measurements depending upon the field orientation. The transitions are mediated by the propagation of 180° or 90° domain walls. The Co two-jump spin switching in the spin-valve structure has contributed to the formation of three stable GMR states: parallel, antiparallel and a new intermediate state.     

Onset of ferromagnetism in ultrathin Fe films on semiconductors

Very thin Fe films have been grown by molecular beam epitaxy on Ge(001), GaAs(001) and ZnSe(001) substrates, under identical preparation conditions. The electronic and magnetic properties of such interfaces have been studied, as a function of the Fe thickness, by means of spin resolved inverse photoemission. From the spin dependence of Fe empty states, we observe the onset of room temperature ferromagnetism to occur at a Fe thickness as low as three monolayers (ML) for Fe/Ge, while 5 and 8 ML have been found for Fe/GaAs and Fe/ZnSe, respectively.     

Spin wave excitations in Fe films grown on GaAs(1 1 3)A substrates

The spin wave excitation and its size effect has been studied in Al-capped Fe films grown on low-symmetry GaAs(1 1 3)A substrates. The temperature dependence of saturation magnetization follows an effective Bloch's law as long as magnetization remains larger than about 70% of its saturation value. A significant increase of the spin wave parameter B is found in Al-capped ultrathin Fe films grown on GaAs(1 1 3)A compared to bulk Fe, Fe films on GaAs(0 0 1) and other systems. This is explained as a result of the reduction in uniaxial magnetic anisotropy observed in this orientation for the same thickness range. However, this observed uniaxial magnetic anisotropy is found to be a likely reason for stabilizing the ferromagnetism.     

Thermal variation and spatial distribution of local magnetization in ultrathin Fe(110) films

Epitaxial ⁵⁷Fe(110) films on W(110) of thicknesses between 7 and 40 Å were studied using in situ CEMS. A bulk-like T3/2 temperature dependence of the hyperfine magnetic field, which measures local magnetization, is observed for all films in the temperature range 90–350 K. The temperature and thickness dependence of magnetization agree with Green function calculations. Spatial distribution of the reduced magnetization is derived from the Mössbauer analysis.     

Magnetic properties of ultrathin Co films on Si (111)

Ultrathin cobalt films on clean (7×7) and Au covered Si (111) substrates were prepared by molecular beam epitaxy. The structure was studied by using scanning tunnelling microscopy and low energy electron diffraction. Magnetic properties were determined with the magneto-optic Kerr effect. It was found that Co nucleates in grains that prefer to grow along the bunched step edges of the Si substrate ([112?] direction), which induces a strong in-plane uniaxial anisotropy. By introducing Au buffer layers, the magnetic characteristics were improved by preventing the silicide reaction between Si and Co. Moreover, the tendency for step decoration disappears gradually results in the in-plane uniaxial anisotropy reduction.     

Exchange bias and anomalous vertical shift of the hysteresis loops in milled Fe/MnO2 material

The present article reports studies on structural and magnetic properties of nanostructured Fe/MnO₂ materials prepared by mechanosynthesis method, with Fe to MnO₂ ratios of 20/80, 50/50 and 60/40. X-ray diffraction patterns indicate that the milled materials have crystalline grain size in the nanoscale region. Mössbauer spectra of the milled materials suggest the presence of two Fe phases for each sample: a nanocrystalline α$\mathrm{\alpha }$-Fe phase with a high degree of disorder/defects and small Fe-oxide particles. The magnetic hysteresis (M(H)$M(H)$) loops, measured at 4.2 K, after the samples were cooled from 300 K in ±10 kOe fields, show unexpected large shifts in both horizontal and vertical directions for the 20/80 sample, while only horizontal shift was detected in the samples with higher Fe concentration. The anomalous vertical shift of the M(H)$M(H)$ loop for the 20/80 sample, observed at low cooling field (10 kOe), is being associated with a large contribution from non-collinear magnetic structure of the particles surface. This surface magnetic contribution is strongly influenced by the field cooling magnitude. A simple model is proposed to interpret this result.