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Controlling exchange bias in Co-CoOx nanoparticles by oxygen content

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 Added by Oscar Iglesias
 Publication date 2009
  fields Physics
and research's language is English




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We report on the occurrence of exchange bias on laser-ablated granular thin films composed of Co nanoparticles embedded in amorphous zirconia matrix. The deposition method allows controlling the degree of oxidation of the Co particles by tuning the oxygen pressure at the vacuum chamber (from 2x10^{-5} to 10^{-1} mbar). The nature of the nanoparticles embedded in the nonmagnetic matrix is monitored from metallic, ferromagnetic (FM) Co to antiferromagnetic (AFM) CoOx, with a FM/AFM intermediate regime for which the percentage of the AFM phase can be increased at the expense of the FM phase, leading to the occurrence of exchange bias in particles of about 2 nm in size. For oxygen pressure of about 10-3 mbar the ratio between the FM and AFM phases is optimum with an exchange bias field about 900 Oe at 1.8 K. The mutual exchange coupling between the AFM and FM is also at the origin of the induced exchange anisotropy on the FM leading to high irreversible hysteresis loops, and the blocking of the AFM clusters due to proximity to the FM phase.



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We present an atomistic model of a single nanoparticle with core/shell structure that takes into account its lattice strucutre and spherical geometry, and in which the values of microscopic parameters such as anisotropy and exchange constants can be tuned in the core, shell and interfacial regions. By means of Monte Carlo simulations of the hysteresis loops based on this model, we have determined the range of microscopic parameters for which loop shifts after field cooling can be observed. The study of the magnetic order of the interfacial spins for different particles sizes and values of the interfacial exchange coupling have allowed us to correlate the appearance of loop asymmetries and vertical displacements to the existence of a fraction of uncompensated spins at the shell interface that remain pinned during field cycling, offering new insight on the microscopic origin of the experimental phenomenology.
Coupling at the interface of core/shell magnetic nanoparticles is known to be responsible for the exchange bias (EB) and the relative sizes of core and shell components are supposed to influence the associated phenomenology. In this work, we have prepared core/shell structured nanoparticles with the total averaged diameter around $sim$ 27 nm and a wide range of shell thicknesses through the controlled oxidation of Co nanoparticles well dispersed in an amorphous silica host. Structural characterizations give compelling evidence of the formation of Co$_3$O$_4$ crystallite phase at the shells surrounding the Co core. Field cooled hysteresis loops display nonmonotonous dependence of the exchange bias $H_E$ and coercive $H_C$ fields, that become maximum for a sample with an intermediate shell thickness, at which lattice strain is also maximum for both the phases. Results of our atomistic Monte Carlo simulations of the particles with the same size and compositions as in experiments are in agreement with the experimental observations and have allowed us to identify a change in the contribution of the interfacial surface spins to the magnetization reversal giving rise to the maximum in $H_E$ and $H_C$.
Some of the main experimental observations related to the occurrence of exchange bias in magnetic systems are reviewed, focusing the attention on the peculiar phenomenology associated to nanoparticles with core/shell structure as compared to thin film bilayers. The main open questions posed by the experimental observations are presented and contrasted to existing theories and models for exchange bias formulated up to date. We also present results of simulations based on a simple model of a core/shell nanoparticle in which the values of microscopic parameters such as anisotropy and exchange constants can be tuned in the core, shell and at the interfacial regions, offering new insight on the microscopic origin of the experimental phenomenology. A detailed study of the of the magnetic order of the interfacial spins shows compelling evidence that most of the experimentally observed effects can be qualitatively accounted within the context of this model and allows also to quantify the magnitude of the loop shifts with striking agreement with the macroscopic observed values.
Au/Co/Au nanopillars fabricated by colloidal lithography of continuous trilayers exhibit and enhanced coercive field and the appearance of an exchange bias field with respect to the continuous layers. This is attributed to the lateral oxidation of the Co interlayer that appears upon disc fabrication. The dependence of the exchange bias field on the Co nanodots size and on the oxidation degree is analyzed and its microscopic origin clarified by means of Monte Carlo simulations based on a model of a cylindrical dot with lateral core/shell structure.
Thin highly epitaxial BiFeO$_3$ films were prepared on SrTiO$_3$ (100) substrates by reactive magnetron co-sputtering. Detailed MOKE measurements on BiFeO$_3$/Co-Fe bilayers were performed to investigate the exchange bias as a function of the films thicknesses and Co-Fe stoichiometries. We found a maximum exchange bias of H$_{mathrm{eb}}$=92 Oe and a coercive field of H$_{mathrm{c}}$=89 Oe for a 12.5 nm thick BiFeO$_3$ film with a 2 nm thick Co layer. The unidirectional anisotropy is clearly visible in in-plane rotational MOKE measurements. AMR measurements reveal a strongly increasing coercivity with decreasing temperature, but no significant change in the exchange bias field.
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