RESUMEN
An accurate description of the local electronic structure is necessary for guiding the design of materials with targeted properties in a controlled way. For complex materials like nanoalloys, self-consistent tight-binding calculations should be a good alternative to ab initio methods, for handling the most complex and large systems (hundreds to thousands of atoms), provided that these parameterized method is well founded from ab initio ones that they intend to replace. Ab initio calculations (density functional theory) enabled us to derive rules for charge distribution as a function of structural change and alloying effects in Co and Pt based systems, from bulk to nanoalloys. A general local neutrality rule per site, orbital and species was found. Based on it, self-consistent tight-binding calculations could be implemented and applied to CoPt nanoalloys. A very good agreement is obtained between tight-binding and DFT calculations in terms of local electronic structure.
RESUMEN
Free-surface-induced L10 chemical long-range ordering phenomena in a nanolayer, a nanowire and a cubic nanoparticle of FePt were studied by means of Monte Carlo simulations. The system was modeled with nearest-neighbor and next-nearest-neighbor interatomic pair interactions deduced from ab initio calculations. The generated samples, the dimensionality of which was determined by appropriate periodic boundary conditions imposed upon the generated supercells, were initially either perfectly ordered in the c-variant L10 superstructure ((001)-oriented monatomic planes), or completely disordered in the fcc crystalline structure. Vacancy-mediated creation of equilibrium atomic configurations was modelled by relaxing the systems at temperatures below the 'order-disorder' transition point using the Glauber algorithm implemented with the vacancy mechanism of atomic migration. The (100)-type-surface-induced heterogeneous nucleation of L10-order domains was observed and quantified by means of an original parameterization enabling selective determination of volume fractions of particular L10-variants. Due to the specific competition between the three kinds of (100)-type free surfaces, the initial c-L10 variant long-range order appeared to be the most stable in the cubic nanoparticle. The initially disordered samples were transformed by the creation of a specific L10 domain structure with a mosaic of particular L10-variant domains at the surfaces and almost homogeneous long-range order in the inner volume. The analysis of correlation effects revealed that chemical ordering was initiated at the free surfaces.
RESUMEN
We report on the development of structural and magnetic order in epitaxially grown L10 FePt thin films. Upon annealing, the easy axis of magnetization changes from the out-of-plain into the in-plain direction. We found that the overall fraction of reoriented domains first increases but after certain time decreases before achieving a saturated state. The results are based on conversion electron Mössbauer spectroscopy studies and confirm Monte Carlo simulations in nano-layered FePt. We present a modified version of the Johnson-Mehl-Avrami (JMA) model adequately describing the experimental findings. Two dynamical processes, the first being a 2D-growth, dominate the initial state of sample annealing and the second being a 3D-growth, dominate the late stage close to saturation. From an Arrhenius plots of JMA coefficients for both processes we extracted the activation energies of the underlying dynamics which are 1.5(1) eV for disordering and 0.8(2) eV for ordering.
