Synthese et caracterisation structurale d'epicouches heterogeenes semiconductrices/ ferromagnetiques: le cas d'agregats de MnP encastres dans une matrice de GaP.

摘要

The general objective of this work is to bring a better understanding of the growth mechanism and the influence of the growth parameters on the microstructure of the heterogeneous magnetic semiconductors layers. Toward this end, we have undertaken a detailed study on the structural characteristics of the GaP:MnP ferromagnetic semiconductor thin films grown by metal organic vapour phase epitaxy (MOVPE). We have focused our effort on three specific objectives: (1) to demonstrate the growth of epitaxial heterogeneous GaP:MnP layers; (2) to establish the influence of the growth parameters on the microstructure of the matrix and nanoclusters; (3) to obtain a detailed structural characterisation of the texture of the clusters as a function of the growth parameters.;We have successfully grown epitaxial heterogeneous GaP:MnP layers without structural defects on GaP substrates at 650°C. The layers contain a uniform ensemble of 15–50 nm quasi-spherical MnP nanoclusters within a dislocation-free GaP epilayer matrix that is fully coherent with the substrate. The clusters occupy 3 to 8% of the total volume of the layer, controlled by the flow of the Mn precursor in the vapor phase. We showed that the growth temperature strongly affect the microstructure of the GaP matrix. At 700°C the surface roughness increases and we have observed 100 nm wide cavities in the GaP matrix. The layers grown at 600°C contain a large density of pile-up defects along GaP{111} facets. To explain these defects we propose the following mechanism: (1) the nucleation of clusters on the GaP growth surface change the morphology of the surrounding matrix; (2) these morphological changes increase the surface roughness and lead to the formation of GaP{111} facets; (3) at 600°C, the probability of the Ga and P atoms to find an epitaxial site on GaP{111} facets is reduced and leads to the formation of pile-up defects.;The detailed microstructural characterization of the GaP:MnP layers have shown that the volume fraction and the dimension of the MnP clusters can be controlled by adjusting the Mn precursor flow rate and the growth temperature, respectively: (1) the volume fraction of the clusters increases with the Mn precursor flow rate; (2) its average dimension increases with the growth temperature. Our work reveals that 80-90% of the clusters were orthorhombic-MnP and 10-20% were hexagonal Mn2P in layer grown at 650°C on GaP(001) substrates. The formation of Mn2P clusters can be reduced by decreasing the growth temperature and can be avoided by growing on GaP(011) substrates.;Our 3D reciprocal space maps measurements have enabled, for the first time, a precise description of the texture of the clusters as a function of the growth temperature, the layer thickness and the substrate orientation. Our results reveal that the orthorhombic MnP nanoclusters are highly textured and distributed in six crystallographic orientation families. They principally grow on GaP(001) and GaP{111} facets with a small fraction of cluster nucleating on higher-index GaP{hhl} facets. Most of epitaxial alignments share a similar component: the MnP(001) plane (c-axis plane) is parallel to the GaP{110} plane family. Along with the diffraction signals indicating specific epitaxial relationships with the substrate, we report the presence of axiotaxial ordering between a certain fraction of the MnP clusters and the GaP matrix.;The texture characterization as a function of the growth parameters revealed that the MnP texture results from a complex growth process, with combined effects of the GaP matrix morphology, the lattice mismatch at the cluster/matrix interface, and the bonding configuration of the GaP seed planes. We propose a qualitative growth model that explains the order of appearance of the various cluster families and the evolution of the proportion of clusters in the different orientations with increasing film thickness. Finally, we have compared the crystallographic orientation of the MnP clusters determined from 3D reciprocal space mapping with those obtained from magnetic measurements. The agreement between the two sets of results confirms that the effective magnetic properties of the heterogeneous layer can be tuned by controlling the texture of the ferromagnetic nanoclusters. (Abstract shortened by UMI.).