Thickness dependence of antiferromagnetic phase transition in Heisenberg-type MnPS3

The behavior of 2-dimensional (2D) van der Waals (vdW) layered magnetic materials in the 2D limit of the few-layer thickness is an important fundamental issue for the understanding of the magnetic ordering in lower dimensions. The antiferromagnetic transition temperature T_N of the Heisenberg-type 2D magnetic vdW material MnPS₃ was estimated as a function of the number of layers. The antiferromagnetic transition was identified by temperature-dependent Raman spectroscopy, from the broadening of a phonon peak at 155 cm⁻¹, accompanied by an abrupt redshift and an increase of its spectral weight. T_N is found to decrease only slightly from ~78 K for bulk to ~66 K for 3L. The small reduction of T_N in thin MnPS₃ approaching the 2D limit implies that the interlayer vdW interaction is playing an important role in stabilizing magnetic ordering in layered magnetic materials.     

Nuclear exchange coupling and electronic structure of low-dimensional semiconductors

We review the nuclear magnetic resonance (NMR) studies of the indirect nuclear exchange coupling and electronic structure of the chain and layered semiconductors Tl(I)M(III)X₂ (M = Tl, Ga, In, X = Se, S, Te) and some other low-dimensional Tl-contained semiconducting compounds. Both univalent and trivalent Tl atoms in these compounds show essential chemical shielding anisotropy despite their formal spherically symmetric 5d¹⁰6s² and 5d¹⁰ electron configurations. Such a behavior results from the sp-hybridization of the Tl electron wave functions. Strong exchange coupling among the spins of Tl¹⁺ and M³⁺ ions, which reside in neighboring chains or layers, is observed. Such coupling is realized due to the overlap of the Tl¹⁺ and M³⁺ electron wave functions across the intervening chalcogen atom. This overlap is the important mechanism in the formation of the valence and conduction bands and determines the electronic structure and properties of the compounds. The long-range indirect nuclear exchange coupling via a chalcogen atom is an analog of the Kramers mechanism of electron spin exchange via a nonmagnetic bridge ion. Recent photoemission spectroscopy studies and band-structure calculations of several aforementioned compounds have confirmed the NMR results on the interchain and interlayer overlap.     

The 2D Rancieite-type manganic acid and its alkali-exchanged derivatives: Part II — Electrochemical behavior

Various layered manganese oxides (phyllomanganates) with the Rancieite structural type were studied for their ability to intercalate lithium in an electrochemical cell. Series of such materials with various interlayer cations (H, Li, Na), various interlayer water contents and various manganese average oxidation states, were investigated, allowing to get precious information on the influence of such key parameters on the electrochemical behavior of phyllomanganates. The water content of electrode materials, different from that of open-air samples, was carefully measured thus allowing to interpret properly electrochemical data. Special attention was given to the first cycles, especially to the influence of an initial charge on the first discharge capacity and on the influence of such electrochemical pretreatment on further intercalation-deintercalation behavior. The electrochemical behavior at first cycles is complex, with the interlayer water playing a major role. Dehydrated materials at T> 200 °C showed a large initial capacity of about 220 mAh/g and a good capacity retention over the ten first discharge-charge cycles.     

Long range ferromagnetism in tunable cobalt(II) layered compounds up to 25 Å apart

We discuss the structure-magnetic property correlations for a series of layered cobalt(II) compounds, derived from the parent host Co(OH)₂. Intercalation takes place by exchange of OH⁻ by organic or inorganic anions resulting in interlayer spacing between 4.65 and 25.4 Å. For all the compounds, ferromagnetic in-plane interaction dominate the magnetic behavior at high temperature, but long range order occurs at low temperature; 3d antiferromagnetic order is observed for small basal spacing and ferromagnetic for large spacing. The nature of the magnetic interaction is discussed briefly.     

Domain size and structure in exchange coupled [Co/Pt]/NiO/[Co/Pt] multilayers

We investigate the competing effects of interlayer exchange coupling and magnetostatic coupling in the magnetic heterostructure ([Co/Pt]/NiO/[Co/Pt]) with perpendicular magnetic anisotropy (PMA). This particular heterostructure is unique among coupled materials with PMA in directly exhibiting both ferromagnetic and antiferromagnetic coupling, oscillating between the two as a function of spacer layer thickness. By systematically tuning the coupling interactions via a wedge-shaped NiO spacer layer, we explore the energetics that dictate magnetic domain formation using high resolution magnetic force microscopy coupled with the magneto-optical Kerr effect. This technique probes the microscopic and macroscopic magnetic behavior as a continuous function of thickness and the interlayer exchange coupling, including the regions where interlayer coupling goes through zero. We see significant changes in domain structure based on the sign of coupling, and also show that magnetic domain size is directly related to the magnitude of the interlayer exchange coupling energy, which generally dominates over the magnetostatic interactions. When magnetostatic interactions become comparable to the interlayer exchange coupling, a delicate interplay between the differing energy contributions is apparent and energy scales are extracted. The results are of intense interest to the magnetic recording industry and also illustrate a relatively new avenue of undiscovered physics, primarily dealing with the delicate balance of energies in the formation of magnetic domains for coupled systems with PMA, defining limits on domain size as well as the interplay between roughness, domains and magnetic coupling.     

Magnetic and electric properties of (Fe,Co)/(Si,Ge) multilayers

We review selected results concerning the interlayer exchange coupling in Fe/Si _x Fe_1−x , Fe/Ge and Co/Si layered structures. Among the ferromagnet/semiconductor systems, Fe/Si structures are the most popular owing to their strong antiferromagnetic interlayer coupling. We show that such interaction depends not only on semiconducting sublayer thickness, but also on deposition techniques and on the chemical composition of the sublayer as well. In similar heterostructures e.g. Fe/Ge, antiferromagnetic coupling was observed only in ion-beam deposited trilayers at low temperatures. In contrast, in Fe/Ge multilayers deposited by sputtering, no such coupling was found. However, when the Ge is partially substituted by Si, antiferromagnetic interlayer coupling appears. For Co/Si multilayers, we observed a very weak exchange coupling and its oscillatory behavior. The growth of Co on Si occurs in an island growth mode. The evolution of magnetic loop shapes can be successfully explained by the interplay between interlayer coupling and anisotropy terms.     

Magnetic phase transition and the corresponding magnetostriction of intermetallic compounds RMnsGe2（R=Sm,Gd）

The temperature dependence of lattice constants a and c of intermetallic compounds RMn₂Ge₂ (R=Sm, Gd) is measured in the temperature range 10－800K by using the x-ray diffraction method. The magnetoelastic anomalies of lattice constants are found at the different kinds of spontaneous magnetic transitions. The transversal and longitudinal magnetostrictions of polycrystalline samples are measured in the pulse magnetic field up to 25T. In the external magnetic field there occurs a first-order field-induced antiferromagnetism－ferromagnetism transition in the Mn sublattice, which gives rise to a large magnetostriction. The magnitude of magnetostrictions is as large as 10^-3. The transversal and longitudinal magnetostrictions have the same sign and are almost equal. This indicates that the magnetostriction is isotropic and mainly caused by the interlayer Mn－Mn exchange interaction. The experimental results are explained in the framework of a two-sublattice ferrimagnet with the negative exchange interaction in one of the sublattices by taking into account the lattice constant dependence of interlayer Mn－Mn exchange interaction.     

The Role of Intermixing in the Phase Determination of the Interlayer Exchange Coupling in Multilayers: Application to Fe-Cr Superlattices

The phase of the short-range interlayer exchange coupling oscillations in Fe n Cr m superlattices is expressed in terms of the intermixing at the Fe-Cr as well as at the Cr-Fe interfaces. The interdiffusion is modeled through stochastic algorithms, which presupposes floating of the atoms on the surface of the sample during the epitaxial growth. It automatically leads to the different chemical and magnetic structure of Fe on Cr and Cr on Fe interfaces. Self-consistent calculations of the magnetic moments are performed on the basis of the periodic Anderson model. Although short-range (2 monolayers (ML)) oscillations of exchange coupling were detected for all considered structures, its amplitude and phase strongly depend on the interface alloying. Introduction of the same intermixing at both interfaces does not change the phase as compared to the ideal superlattices with sharp interfaces. However different interdiffusion leads to the ~ -phase shift in accordance with experimental results for the Fe-Cr-Fe trilayers grown on an Fe whiskers. Distribution of magnetic moments on Fe atoms contains several distinct peaks but their position and relative area weakly depend on the alloying and interlayer exchange coupling in the superlattice. On the contrary, magnetic moments on Cr atoms are very sensitive to the intermixing and their behavior determines the strength and the phase of exchange coupling oscillations.     

Multilayer structures of the iron/chromium type with almost ideal interfaces in an external magnetic field

The magnetic phase diagram of the Fe/Cr/Fe three-layer structure with almost ideal interlayer boundaries was constructed. The effective interlayer interaction in this structure was described by the “half-angle coupling” model. Various system configurations were analyzed taking into account crystalline anisotropy, and the ground state of the system was determined. The behavior of the structure in an external magnetic field applied along easy and hard magnetic axes was studied. The magnetization curves M(H) characteristic of structures with various interface roughness parameter and interlayer exchange values were described and analyzed. The experimental situation is discussed.     

Magnetic phase transitions in layered intermetallic compounds

Magnetic, magnetoelastic, and magnetotransport properties have been studied for the RMn₂Si₂ and RMn₆Sn₆ (R is a rare earth metal) intermetallic compounds with natural layered structure. The compounds exhibit wide variety of magnetic structures and magnetic phase transitions. Substitution of different R atoms allows us to modify the interatomic distances and interlayer exchange interactions thus providing the transition from antiferromagnetic to ferromagnetic state. Near the boundary of this transition the magnetic structures are very sensitive to the external field, temperature and pressure. The field-induced transitions are accompanied by considerable change in the sample size and resistivity. It has been shown that various magnetic structures and magnetic phase transitions observed in the layered compounds arise as a result of competition of the Mn–Mn and Mn–R exchange interactions.     

Ni adsorbate dynamics on a NiO(0 0 1) surface

We present results concerning the dynamical behavior of a Ni³⁺ adsorbate on a NiO(0 0 1) surface obtained by molecular dynamics simulations. In a first place, we examined at low temperature the position of the Ni³⁺ ion as an adatom on the surface and the corresponding modification of its local environment as reflected on the pair-wise radial distribution function. The calculation of the vibrational properties of the adatom by means of the phonon local density of states (LDOS) shows that there is an anisotropic behavior both in the two principal in-plane directions as well as in the direction normal to the surface in accordance with the structural results. We compare the phonon LDOS of the Ni³⁺ adatom with the corresponding results for the Ni²⁺ adatom and the Ni²⁺ surface cations.Static energetic calculations are indicative that the exchange of the Ni³⁺ ion with a surface Ni²⁺ ion could be favorable. Such a behavior is confirmed by results observed at temperatures higher than 700 K where the Ni³⁺ adsorbate is located on a substitutional position on the surface and not on adatom position. The exchange takes place through simple or double exchange mechanisms. The structural and dynamical behavior of the Ni³⁺ ion at the substitution position was investigated in the temperature range 700-2000 K through the calculation of the pair distribution function, the relaxed interlayer relative position (RIRP), mean-square displacements (MSDs) and phonon LDOS. Results show that in comparison with the Ni²⁺ surface ions the Ni³⁺ ion at substitution position is more tightly bound especially in the direction normal to the surface as is indicated by the local structure and the contraction it presents as well as its phonon LDOS. As temperature increases the binding of the Ni³⁺ ion becomes less important as reflected on the physical properties mentioned above.     

Critical behavior and spatial crossover in the frustrated antiferromagnetic Heisenberg model on a triangular lattice

The critical properties of the three-dimensional frustrated Heisenberg model on a layered triangular lattice with variable interplane exchange interaction have been investigated by the replica Monte Carlo method. All main magnetic and chiral critical exponents have been calculated. It is found that a decrease in the interlayer exchange leads to crossover from the three-to two-dimensional critical behavior.     

Soft X-ray resonant magnetic scattering study of magnetization reversal in low dimensional magnetic heterostructures

Soft X-ray resonant magnetic scattering (SXRMS) has been used to investigate the microscopic magnetization reversal behavior of complex magnetic systems. SXRMS is a unique technique, providing chemical, spatial and magnetic sensitivity, which is not affected by external magnetic fields. The study of two selected thin magnetic heterostructures is presented, amorphous rare-earth transition metal alloys and perpendicular exchange coupled antiferromagnetic/ferromagnetic films. In the first system, the internal structure of magnetic stripe domains on nanometer length scales is obtained by measuring bi-dimensional (2D) scattering images. In the second system, the element specificity is exploited to identify the role of the uncompensated spins in the antiferromagnetic layer on the exchange coupling phenomena. Future trends are also discussed.     

MAGNETIC POLARIZATION OF Pd SPACERS AND OSCILLATORY EXCHANGE COUPLING BETWEEN Fe AND Pd LAYERS IN Fe/Pd MULTILAYERS

Ay oscillatory behavior in specific saturation magnetization of Fe/Pd multilayers is observed. The conversion electron M?ssbauer spectroscopy and other experiments indicate that this behavior is caused by the magnetic polarization of Pd spacers, which alternates between positive and negative polarization with respect to the magnetic moments of Fe layers. The interlayer coupling between two Fe layers always keeps ferromagnetic. Then, the interlayer couplings in ferromagnetic metal/nearly ferromagnetic metal multilayers were calculated By using the model of Barnas. The results of calculation prove that the above phenomenon might appear under some condition. The influence of magnetic polarization potential of spacers and interface chemical potential on the interlayer couplings is also discussed.     

Static critical behavior of 3D frustrated Heisenberg model on stacked triangular lattice with variable interlayer exchange coupling

Several Monte Carlo algorithms are used to examine the critical behavior of the 3D frustrated Heisenberg model on stacked triangular lattice with variable interlayer exchange coupling for values of the interlayer-to-intralayer exchange ratio R = |′/J| in the interval between 0.01 and 1.0. A finite-size scaling technique is used to calculate the static magnetic and chiral critical exponents α (specific heat), γ and γ_k (susceptibility), β and β_k(magnetization), ν and ν_k(correlation length), and the Fisher exponent η. It is shown that 3D frustrated Heisenberg models on stacked triangular lattice with R > 0.05 constitute a new universality class of critical behavior. At lower R, a crossover from 3D to 2D critical behavior is observed.     

Thin-Film Three-Layer Fe/Poly(diphenylene phthalide)/Fe Systems: Structural Properties and Behavior in Magnetic Fields

The structural and magnetic properties of thin-film Fe/poly(diphenylene phthalide) (PDP)/Fe systems are studied, along with the behavior of these systems in magnetic fields. The mean surface roughness of the studied samples is around 5–8 nm, and local near-surface magnetic properties show variation within 10%. The samples are characterized by two-step hysteresis loops, the step size depending on the thickness of the polymer layer and the difference in the thickness between the magnetic layers. The results are explained by the effects the exchange interaction between the magnetic layers, mediated by the PDP interlayer, has on the behavior of our samples in a magnetic field.     

Magnetism of Co layers in a Co/Si multilayer film

The magnetic properties of Co/Si multilayer films produced through rf ion sputtering were studied in the temperature range 4.2–300 K. The dependences of the spontaneous magnetization and hysteresis characteristics of the films on the thicknesses of the magnetic layers and nonmagnetic spacers are established. It is shown that these dependences are determined to a large extent by interlayer interfaces, in which the effective magnetic moment of the Co atoms and the exchange interaction decrease and magnetic-anisotropy dispersion arises. A probable cause of the interface formation is interlayer mixing (which is estimated to penetrate to a depth of 15 Å) and the strong effect of Si on the Co electronic structure.     

Ion irradiation of exchange bias systems for magnetic sensor applications

It has been demonstrated that He⁺ ion irradiation is an excellent tool for modifying magnetic properties, like the magnetic anisotropy, the interlayer exchange coupling strength and the exchange bias field of ultra-thin magnetic layered systems. This paper summarizes the effects of ion irradiation on exchange bias systems. As a first example, for possible applications of the ion induced magnetic effects, the realization of an angle sensing device is described. Received: 11 November 2002 / Accepted: 12 November 2002 / Published online: 4 April 2003 RID="*" ID="*"Corresponding author. Fax: +49-631-205-4095, E-mail: fassbend@physik.uni-kl.de RID="**" ID="**"Present address: Université de Rouen, Rouen, France     

Coupling Stacking Orders with Interlayer Magnetism in Bilayer H-VSe_2

Stacking-dependent magnetism in van der Waals materials has caught intense interests.Based on the first principle calculations,we investigate the coupling between stacking orders and interlayer magnetic orders in bilayer H-VSe_2.It is found that there are two stable stacking orders in bilayer H-VSe_2,named AB-stacking and A'B-stacking.Under standard DFT framework,the A'B-stacking prefers the interlayer AFM order and is semiconductive,whereas the AB-stacking prefers the FM order and is metallic.However,under the DFT+U framework both the stacking orders prefer the interlayer AFM order and are semiconductive.By detailedly analyzing this difference,we find that the interlayer magnetism originates from the competition between antiferromagnetic interlayer super-superexchange and ferromagnetic interlayer double exchange,in which both the interlayer Se-4p_z orbitals play a crucial role.In the DFT+U calculations,the double exchange is suppressed due to the opened bandgap,such that the interlayer magnetic orders are decoupled with the stacking orders.Based on this competition mechanism,we propose that a moderate hole doping can significantly enhance the interlayer double exchange,and can be used to switch the interlayer magnetic orders in bilayer VSe_2.This method is also applicable to a wide range of semiconductive van der Waals magnets.