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INVESTIGATION OF Ge SURFACE DIFFUSION AND SiGe NANOSTRUCTURES BY SPECTRO-MICROSCOPY TECHNIQUES

Abstract : SiGe nanostructures on crystalline Si substrates with (001) orientation are among the most studied system in condensed matter physics and nanoscience. This interest has been mainly driven by the important potential applications in opto and nano-electronic devices thanks to the improvement of the optical and electronic properties compared to bulk systems. These features come essentially from the possibility of engineering the strain field within the nanostructures using the lattice mismatch of ~ 4 % between Ge and Si and from the spatial confinement, capable of modifying the electronic band structure leading to an increase of the charge carrier mobility. It is obvious that these applications largely depend on the control of surface processes during the growth of the nanostructures, and their performance are strongly dependent on strain relaxation and dislocation injection. Besides the technological interest, the SiGe/Si(001) system has received much attention since it is also a model for understanding the fundamental processes occurring during 3D island formation and self-organization phenomena. In fact, the lattice mismatch between Ge and Si introduces a stress field which has dramatic effects on the growth process and is responsible for a number of structural and electronic phenomena. In particular, the stored elastic energy can be partially relieved by spontaneous formation of 3D objects of nanometric size on top of a pseudomorphic SiGe wetting layer. This growth mode, called Stranski-Krastanov (SK), is a way of easily forming self-assembled nanostructures, which can be used to obtain quantum confinement of charge carriers in nanoelectronics device applications. In recent years, considerable efforts have been devoted to the growth of hetero-epitaxial SiGe nanostructures with well controlled size, shape and positioning, and with defined stoichiometry and strain state. However, some aspects still need to be addressed for a complete understanding of this system, including: (i) the competition between kinetic and thermodynamic factors for island formation, (ii) the mechanisms governing the relative growth of individual nanostructures, (iii) the interplay between SiGe intermixing and strain relaxation mechanisms. In the present work, we carry out an experimental investigation of the relationship between morphology, elemental composition, strain state and electronic structure of self-assembled and lithographically defined SiGe nanostructures by means of several spectro-microscopy techniques. The Si and Ge diffusion dynamics and the self-organization phenomena during the growth of SiGe islands have been studied by Scanning Auger Microscopy (SAM) and Atomic Force Microscopy (AFM). Micro-Raman, SAM and Scanning Transmission Electron Microscopy coupled with Electron Energy Loss Spectroscopy (STEM-EELS) techniques have been used for the investigation of the interplay between strain relaxation mechanisms and SiGe intermixing in self-assembled islands. The effects of strain and composition on the electronic band structure in lithographically defined SiGe nanostructures, in layout very close to those used in prototype devices, have been characterized with nanoscale spatial resolution joining information from Tip Enhanced Raman Spectroscopy (TERS), nanofocused X-Ray Diffraction (XRD) and Energy-Filtered PhotoElectron Emission Microscopy (PEEM). The thesis is conceptually divided in two main parts: the first, to which belong Chapters 1, 2 and 3, deals with the experimental investigation of the Ge surface diffusion and of the self-organization phenomena of SiGe islands grown in a bottom-up approach; the second, including Chapters 4 and 5, is based on the experimental characterization of the strain state and of the strain-induced effects on the electronic band structure of lithographically defined SiGe nanostructures obtained in a top-down approach Chapter 1 presents an overview on the basic processes occurring during hetero-epitaxial growth of thin solid films. In the Chapter 2 the surface diffusion of Ge on a clean and C covered Si(001) surface promoted by annealing at high temperatures in UHV of pure Ge stripes is experimentally investigated by means of in-situ Scanning Auger Microscopy. The influence of a controlled carbon coverage on the Ge surface diffusion is quantitatively studied, showing that the diffusion coefficient presents a strong dependence on carbon coverage (see Fig. 1(a)). Chapter 3 deals with the experimental investigation of the growth process of self-assembled SiGe islands on Si(001) (see Fig. 1(b)). From the size and density evolution exhibited by the nucleated islands, we propose a scenario where the island growth is essentially driven by kinetic factors within a diffusion limited regime. Finally, we investigated the interplay among SiGe intermixing and plastic relaxation, showing that the surface thermal diffusion growth method leads to the formation of coherent islands (dislocation-free), as shown in Fig. 1(c), larger than those attainable by MBE and CVD. Chapter 4 presents the mapping with nanoscale resolution of strain, composition, local work function and valence band structure of lithographically defined SiGe embedded nano-stripes using TERS and Energy-Filtered PEEM (see Fig. 1(d) showing the Ge concentration mapping of the nano-stripes as obtained by PEEM analysis). In Chapter 5 are presented the first results of a direct characterization of the strain state of lithographically defined SiGe nano-ridges using the recently developed nanofocused XRD technique. The work presented in this thesis is the outcome of an experimental PhD research project developed at the Politecnico di Milano (Milano, Italy) in co-tutorship with the École Polytechnique (Paris, France) and the French Atomic Energy Commission (CEA-Saclay, France). SAM and AFM have been performed at Department of Physics of the Politecnico di Milano. Micro-Raman Spectroscopy has been carried out at the Materials Science Department of the Università Milano-Bicocca. PEEM measurements have been realized at CEA and during two standard experimental runs at the TEMPO beamline of SOLEIL Synchrotron (France). TERS and preliminary TEM analysis have been performed at the École Polytechnique, while more extensive TEM and STEM-EELS measurements have been developed at IMM-CNR in Catania. The nano-XRD experiment has been carried out during a standard experimental run at ID13 beamline of the European Synchrotron Radiation Facility (ESRF). The close collaboration with the laboratory L-NESS in Como made available the set of the lithographically-defined investigated samples. The experimental results have been exploited in close collaboration with a theory group at the Materials Science Department of the Università Milano-Bicocca for a deeper insight into the atomic level mechanisms during island growth process.
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Giovanni Maria Vanacore. INVESTIGATION OF Ge SURFACE DIFFUSION AND SiGe NANOSTRUCTURES BY SPECTRO-MICROSCOPY TECHNIQUES. Materials Science [cond-mat.mtrl-sci]. Politecnico di Milano; Ecole Polytechnique X, 2011. English. ⟨tel-00725427⟩

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