Surface effects in nanoparticles: application to maghemite -Fe O

We present a microscopic model for nanoparticles, of the maghemite (-Fe₂O₃) type, and perform classical Monte Carlo simulations of their magnetic properties. On account of M?ssbauer spectroscopy and high-field magnetisation results, we consider a particle as composed of a core and a surface shell of constant thickness. The magnetic state in the particle is described by the anisotropic classical Dirac-Heisenberg model including exchange and dipolar interactions and bulk and surface anisotropy. We consider the case of ellipsoidal (or spherical) particles with free boundaries at the surface. Using a surface shell of constant thickness ( nm) we vary the particle size and study the effect of surface magnetic disorder on the thermal and spatial behaviors of the net magnetisation of the particle. We study the shift in the surface “critical region” for different surface-to-core ratios of the exchange coupling constants. It is also shown that the profile of the local magnetisation exhibits strong temperature dependence, and that surface anisotropy is responsible for the non saturation of the magnetisation at low temperatures. Received 1 September 1999 and Received in final form 3 November 1999     

Interfacial polarisation effect on the interlayer couplings in Co/Rh sandwiches

The structural, magnetic and transport properties of Co/Rh sandwiches grown by ultra high vacuum evaporation and sputtering have been studied. High-energy electron diffraction observations during the growth reveal that both Co and Rh layers have been stabilised in the (111) fcc structure for the evaporated sandwiches. X-ray measurements performed on sputtered samples show a predominant fcc polycrystalline structure of the stacks with a preferential (111) texture. Magnetisation and magnetoresistance measurements show a very strong antiferromagnetic exchange coupling for thin Rh layers, reaching for 4.8? Rh, the strongest ever observed in exchange coupled systems. This value is in good agreement with the value of obtained by ab initio calculations for Co/Rh (hcp) superlattices. This is explained by the magnetic nature of the Co/Rh interfaces. Indeed, the variation of the measured saturation magnetisation as a function of the Co layer thickness shows no evidence of Co moment reduction for the Co atoms located at the interfaces, even for the very thin layers. The value of the preserved magnetic moments of the cobalt atoms at the interfaces is confirmed by ab initio calculations for Co/Rh superlattices taking the intermixing into account. Received: 18 February 1998 / Received in final form: 30 April 1998 / Accepted: 29 May 1998     

Spontaneous surface magnetisation of single crystal MnF2 in the antiferromagnetic state

Spontaneous magnetisation of (100) and (010) surfaces of single crystal MnF₂ in the antiferromagnetic state has been discovered. The sign of the surface magnetisation is determined by the difference in dielectric constants of MnF₂ and ambient matter: magnetisation is directed to the substance with smaller . Received 28 August 1998 and Received in final form 15 December 1998     

A numerical study of the formation of magnetisation plateaus in quasi one-dimensional spin-1/2 Heisenberg models

We study the magnetisation process of the one-dimensional spin-1/2 antiferromagnetic Heisenberg model with modulated couplings over j=1,2,3sites. It turns out that the evolution of magnetisation plateaus depends on j and on the wave number q of the modulation according to the rule of Oshikawa et al. A mapping of two- and three-leg zig-zag ladders on one-dimensional systems with modulated couplings yields predictions for the occurrence of magnetization plateaus. The latter are tested by numerical computations with the DMRG algorithm. Received 14 October 1999 and Received in final form 6 January 2000     

Form-factor measurements on chromium with high-energy synchrotron radiation

Results of high-energy magnetic X-ray diffraction on pure antiferromagnetic chromium are presented. The temperature dependence of the propagation vector of the spin-density wave (SDW) and the strain-wave (SW) could be reproduced. The temperature dependence of the magnetic integrated intensity could be measured in the transversally as well as in the longitudinally polarised SDW phase. The magnetic form-factor has been determined in the transversally polarised SDW phase with five magnetic satellites. For the first time a spin-orbit separation has been performed by comparing X-ray to neutron data. The small orbital contribution to the magnetisation density turns out to be negligible, in agreement to our relativistic band-structure calculations. In addition, measurements of strain-wave reflections have been undertaken, and the results complement previous studies. Received 17 August 1998 and Received in final form 10 August 1999     

Interplay between chains of S = 5/2 localised spins and two-dimensional sheets of organic donors in the synthetically built magnetic multilayer λ ‒ (BETS)2FeCl4

In order to understand the magnetic field-induced restoration of a highly conductive state in , static (SQUID) and dynamic (ESR and AFR) magnetization measurements were performed on polycrystalline samples and single crystals, respectively. In addition, cantilever and resistivity measurements under steady fields were performed. While the metal-insulator transition curve of the () phase diagram exhibits a first order character, a “spin-flop” transition line divides the insulating state when the magnetic field is applied along the easy axis of magnetization. The effects of a RKKY-type indirect exchange and of applied magnetic field are described within the framework of a generalized Kondo lattice, namely two chains of localised spins coupled through the itinerant spins of the 2D sheets of BETS. The calculations, which can incorporate intramolecular electron correlations within a mean field theory, are in qualitative agreement with the field induced transition from the antiferromagnetic insulating ground state to a canted one, i.e. a not fully oriented paramagnetic, but metallic state. Received: 6 August 1997 / Received: 5 November 1997 / Accepted: 10 November 1997     

Experimental attempts to measure non-collinear local magnetisation

Representing atomic magnetic moments as simple vectors has limitations when applied to systems in which orbital moments, or significant spin-orbit coupling is present. These phenomena are associated with interactions leading to non-collinearity in the magnetisation distribution. Several experimental techniques are available to probe such non-collinearity. The most direct is to measure both the magnitude and direction of the magnetic interaction vectors, which give its Fourier components. Such measurements are now becoming possible for antiferromagnets with the advent of a new generation of neutron polarimeters, which will allow both greater geometric flexibility and higher precision. However, up to now non-collinear magnetisation distributions have been revealed by more indirect means. Polarised neutron flipping ratio measurements can give only a single component of the magnetic interaction vector directly. However, the special geometric properties of the interaction vector and the symmetry breaking properties of an applied field can be exploited to obtain evidence of non-collinearity in the magnetisation distribution even from such limited data.     

Magnetic relaxation phenomena in a CuMn spin glass

Experiments on the temperature and time dependence of the response function and the field cooled magnetisation of a Cu(Mn) spin glass at temperatures below the zero field spin glass temperature are used to explore the non-equilibrium nature of the underlying spin configuration. The results imply that a certain spin configuration is imprinted on the system as the temperature is decreased at a constant cooling rate. The cooling rate governs the magnitude of the FC magnetisation ((H,T)). Any intermittent halt at a constant temperature, , imprints an extended spin configuration, a process that is reflected e.g. in a downward relaxation of . On continued cooling at the same rate, the magnitude of (T) remains at a lower level than that of a continuous cooling curve. These results are put into the context of the corresponding behaviour of the response function as observed in measurements of the relaxation of the zero field cooled magnetisation. Received 27 October 1998 and Received in final form 30 November 1998     

Probing the anisotropy constants of SmCo5 and PrCo5 by Hall resistance measurements in pulsed high magnetic fields up to 47 T

In order to assess the anisotropy constants of highly anisotropic thin film samples with anisotropy fields well above 10 T, Hall resistance measurements were conducted in pulsed magnetic fields. These measurements also deliver the anomalous Hall data, which are proportional to the perpendicular magnetisation. This specific approach combines the high field values obtainable by pulsed fields with a measurement technique sensitive enough to be applied to thin film samples. Two epitaxial Rare Earth-Cobalt thin films with large in-plane uniaxial magnetocrystalline anisotropy at room temperature were studied. The resulting anisotropy fields and constants are discussed with respect to measurements on single crystals and similar films investigated in quasi-static magnetic fields well below the anisotropy field. The present technique proved to be very valuable to highly anisotropic samples, as the approach to saturation is fully monitored and the data thus provides a more extended view on the hard axis magnetisation process.     

Antiferromagnetic resonance and high magnetic field properties of NaNiO2

Magnetisation measurements up to 23 T and submillimeter wave ESR in the frequency region 48-380 GHz have been performed on NaNiO₂ powders at low temperature. Also typical spectra above the Néel temperature are shown. At 4 K the magnetisation shows a spin-flop transition at 1.8 T and saturation at 10 T. /Ni confirms the low spin state of the Ni³⁺ ions. The susceptibility exhibits a maximum at K with and K. NaNiO₂ is an A-type antiferromagnet: we derive K and K for the interactions between Ni ions within and between adjacent layers, respectively. The AFMR spectra yield an energy gap of 52.5 GHz, in agreement with the spin-flop value derived from the magnetisation. The anisotropy of the g factor observed at 100 K with can be attributed to the Jahn-Teller effect for Ni³⁺ ions in the low spin state, which stabilises the occupation. We finally comment on the isomorphic controversial Li_1-xNi_1+xO₂ compound. Received 9 March 2000 and Received in final form 13 July 2000.     

Charge-density-wave instabilities and quantum transport in the monophosphate tungsten bronzes with m = 5 alternate structure

Resistivity, thermoelectric power and magnetotransport measurements have been performed on single crystals of the quasi two-dimensional monophosphate tungsten bronzes (PO₂)₄(WO₃)_2m for m =5 with alternate structure, between 0.4 K and 500 K, in magnetic fields of up to 36 T. These compounds show one charge density instability (CDW) at 160 K and a possible second one at 30 K. Large positive magnetoresistance in the CDW state is observed. The anisotropic Shubnikov-de Haas and de Haas-van Alphen oscillations detected at low temperatures are attributed to the existence of small electron and hole pockets left by the CDW gap openings. Angular dependent magnetoresistance oscillations (AMRO) have been found at temperatures below 30 K. The results are discussed in terms of a weakly corrugated cylindrical Fermi surface. They are shown to be consistent with a change of the Fermi surface below 30 K. Received 23 November 1999 and Received in final form 23 March 2000     

Magnons localised on surface steps: a theoretical model

We present the solution of the full magnetic problem arising from the absence of magnetic translation symmetry in two dimensions due to an extended magnetic surface step on the surface boundary of an insulating magnetic substrate. The calculation concerns in particular the spin fluctuation dynamics of a magnetic atomic step in the surface of a ferromagnetic simple cubic lattice, the spin order being in the direction normal to surface boundary. Only exchange interactions are considered between the spins in the model. The theoretical approach determines the evanescent spin fluctuation field in the two dimensional plane normal to the direction of the step edge. This field arises owing to the absence of magnetic translation symmetry in this plane, and is completely independent of the form of the surface defect, underlying the general character of the calculation. We show the existence of optical localised magnon modes propagating along the step, their fields being evanescent in the plane normal to the step direction. Received 17 February 1999     

Incommensurate modulated magnetic structure in orthorhombic EuPdSb

Orthorhombic EuPdSb is known to undergo two magnetic transitions, at 12 K and at T _N≃ 18 K, and in phase III (T < 12 K), single crystal magnetisation data have shown that the spin structure is collinear antiferromagnetic, with magnetic moments along the crystal a axis. From a ¹⁵¹Eu M?ssbauer absorption study, we show that, at any temperature within phase III, all the moments have equal sizes, and that in phase II (12 K< T <18 K) the magnetic structure is modulated and incommensurate with the lattice spacings. The modulation is close to a pure sine-wave just below T _N = 18 K, and it squares up as temperature is lowered. We measured the thermal variations of the first and third harmonics of the moment modulation, and we could determine the first and third harmonics of the exchange coupling. We furthermore show that the antiferromagnetic-incommensurate transition at 12 K is strongly first order, with a hysteresis of 0.05 K, and that the incommensurate-paramagnetic transition at 18 K is weakly first order. Finally, we present an explanation of the spin-flop transition observed in the single crystal magnetisation data in phase III when || in terms of an anisotropic molecular field tensor. Received 17 January 2001 and Received in final form 20 March 2001     

Magnetostructural transition in NdCu2

The magnetic (H , T)-phase diagram of the orthorhombic compound NdCu₂ was investigated for external magnetic fields up to 15 T parallel to the crystallographic c-direction. Magnetization and magnetostriction measurements reveal an anomalous change of the magnetic properties as well as giant magnetostriction (GMS) and large hysteretic effects. This behaviour is similar to that observed in some other RCu₂ compounds where it has been interpreted as a conversion of the magnetic Ising axis. In contrast to these other RCu₂ compounds, however, the easy axis of magnetization in NdCu₂ is the b-axis. The macroscopic measurements are compared with neutron diffraction experiments which reveal GMS along the b-axis and a new magnetic phase with propagation vector in the converted crystal. Received 27 March 2000 and Received in final form 11 September 2000     

High magnetic field properties and ESR of the compounds

compounds have a layered structure made of alternating Ni-O and Li-O slabs. An amount z of extra divalent Ni ions is always present in the Li-O layers. We show, using high field magnetisation, static and dynamic susceptibility and high frequency ESR, that the magnetic properties are driven by the z parameter. The compounds can be described as ferromagnetic Ni-O layers, bridged by clusters possessing a net ferromagnetic moment. Received: 24 July 1998 / Revised and Accepted: 23 September 1998     

A generalized spin ladder in a magnetic field

We study the phase diagram of coupled spin-1/2 chains with bilinear and (chiral) three-spin exchange interactions in a magnetic field. The model is soluble on a one-parametric line in the space of coupling constants connecting the limiting cases of a single and two decoupled Heisenberg chains with nearest neighbour exchange only. We give a complete classification of the low-energy properties of the integrable system and introduce a numerical method which allows to study the possible phases of spin ladder systems away from the soluble line in a magnetic field. Received 17 November 1998 and Received in final form 22 January 1999     

Ising films with surface defects

The influence of surface defects on the critical properties of magnetic films is studied for Ising models with nearest-neighbour ferromagnetic couplings. The defects include one or two adjacent lines of additional atoms and a step on the surface. For the calculations, both density-matrix renormalization group and Monte Carlo techniques are used. By changing the local couplings at the defects and the film thickness, non-universal features as well as interesting crossover phenomena in the magnetic exponents are observed. Received 27 July 2000 and Received in final form 5 October 2000     

Macroscopic and local magnetic moments in Si-doped CuGeO 3 as determined by neutron and μSR studies

The temperature-concentration phase diagram of the Si-doped spin-Peierls compound CuGeO₃ is investigated by means of neutron scattering and muon spin rotation spectroscopy in order to determine the microscopic distribution of the magnetic and lattice dimerised regions as a function of doping. The analysis of the zero-field muon spectra has confirmed the spatial inhomogeneity of the staggered magnetisation that characterises the antiferromagnetic superlattice peaks observed with neutrons. In addition, the variation of the macroscopic order parameter with doping can be understood by considering the evolution of the local magnetic moment as well as of the various regions contributing to the muon signal. Received 6 September 2000 and Received in final form 29 January 2001     

Low temperature Kondo reduction of quadrupolar and magnetic moments in the YbCuAl series

We present measurements in the YbCu_5-xAl_x series, down to the 50 mK range, using ¹⁷⁰Yb M?ssbauer absorption spectroscopy and magnetisation measurements. In this series, the hybridisation between the Yb 4 f electrons and the conduction electrons is known to decrease as the Al content x increases. We apply the variational solution of the impurity Kondo problem to the interpretation of our data. We show that the Kondo temperature can be derived from the measured 4 f quadrupole moment and, for the magnetically ordered compounds (), we obtain the exchange energy as a function of the Al content. Our findings are in general agreement with Doniach's model describing the onset of magnetic ordering according to the relative values of the Kondo and exchange energy scales. Received 16 April 1998     

Quantum spin model of a cubic ferromagnet in a magnetic field

The zero temperature phase diagram of a one-dimensional ferromagnet with cubic single ion anisotropy in an external magnetic field is studied. The mean-field approximation and the density-matrix renormalization group method are applied. Two phases at finite magnetic fields are identified: a canted phase with spontaneously broken symmetry and a phase with magnetization along the magnetic field. Both methods predict that the canted phase exists even for the single-ion anisotropy strong enough to destroy the magnetic order at zero magnetic field. In contrast to the mean-field theory, the density-matrix renormalization group predicts a reentrant behavior for the model. The character of the phase transition at finite magnetic field has also been considered and the critical index has been found. Received 9 May 2000 and Received in final form 5 July 2000