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Register a new userKinetic Control of Morphology and Composition in Ge/GeSn Core/Shell Nanowires
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The growth of Sn-rich group-IV semiconductors at the nanoscale provides new paths for understanding the fundamental properties of metastable GeSn alloys. Here, we demonstrate the effect of the growth conditions on the morphology and composition of Ge/GeSn core/shell nanowires by correlating the experimental observations with a theoretical interpretation based on a multi-scale approach. We show that the cross-sectional morphology of Ge/GeSn core/shell nanowires changes from hexagonal to dodecagonal upon increasing the supply of the Sn precursor. This transformation strongly influences the Sn distribution as a higher Sn content is measured under the {112} growth front. Ab-initio DFT calculations provide an atomic-scale explanation by showing that Sn incorporation is favored at the {112} surfaces, where the Ge bonds are tensile-strained. A phase-field continuum model was developed to reproduce the morphological transformation and the Sn distribution within the wire, shedding light on the complex growth mechanism and unveiling the relation between segregation and faceting. The tunability of the photoluminescence emission with the change in composition and morphology of the GeSn shell highlights the potential of the core/shell nanowire system for opto-electronic devices operating at mid-infrared wavelengths.
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Strain engineering in Sn-rich group IV semiconductors is a key enabling factor to exploit the direct band gap at mid-infrared wavelengths. Here, we investigate the effect of strain on the growth of GeSn alloys in a Ge/GeSn core/shell nanowire geometry. Incorporation of Sn content in the 10-20 at.% range is achieved with Ge core diameters ranging from 50nm to 100nm. While the smaller cores lead to the formation of a regular and homogeneous GeSn shell, larger cores lead to the formation of multi-faceted sidewalls and broadened segregation domains, inducing the nucleation of defects. This behavior is rationalized in terms of the different residual strain, as obtained by realistic finite element method simulations. The extended analysis of the strain relaxation as a function of core and shell sizes, in comparison with the conventional planar geometry, provides a deeper understanding of the role of strain in the epitaxy of metastable GeSn semiconductors.
General expressions for the electron- and hole-acoustical-phonon deformation potential Hamiltonian (H_{E-DP}) are derived for the case of Ge/Si and Si/Ge core/shell nanowire structures (NWs) with circular cross section. Based on the short-range elastic continuum approach and on derived analytical results, the spatial confined effects on the vector phonon displacement, the phonon dispersion relation and the electron- and hole-phonon scattering amplitudes are analyzed. It is shown that the acoustical vector displacement, phonon frequencies and H_{E-DP} present mixed torsional, axial, and radial components depending on the angular momentum quantum number and phonon wavector under consideration. The treatment shows that bulk group velocities of the constituent materials are renormalized due to the spatial confinement and intrinsic strain at the interface. The role of insulating shell on the phonon dispersion and electron-phonon coupling in Ge/Si and Si/Ge NWs are discussed.
We settle a general expression for the Hamiltonian of the electron-phonon deformation potential (DP) interaction in the case of non-polar core-shell cylindrical nanowires (NWs). On the basis of long range phenomenological continuum model for the optical modes and by taking into account the bulk phonon dispersions, we study the size dependence and strain-induced shift of the electron-phonon coupling strengths for Ge-Si and Si-Ge NWs. We derive analytically the DP electron-phonon Hamiltonian and report some numerical results for the frequency core modes and vibrational amplitudes. Our approach allows for the unambiguous identification of the strain and confinement effects. We explore the dependence of mode frequencies and hole-DP scattering rates on the structural parameters of these core-shell structures, which constitute a basic tool for the characterization and device applications of these novel nanosystems.
We model shell formation of core-shell noble metal nanoparticles. A recently developed kinetic Monte Carlo approach is utilized to reproduce growth morphologies realized in recent experiments on core-shell nanoparticle synthesis, which reported smooth epitaxially grown shells. Specifically, we identify growth regimes that yield such smooth shells, but also those that lead to the formation of shells made of small clusters. The developed modeling approach allows us to qualitatively study the effects of temperature and supply the shell-metal atoms on the resulting shell morphology, when grown on a pre-synthesized nanocrystal core.
We define single quantum dots of lengths varying from 60 nm up to nearly half a micron in Ge-Si core-shell nanowires. The charging energies scale inversely with the quantum dot length between 18 and 4 meV. Subsequently, we split up a long dot into a double quantum dot with a separate control over the tunnel couplings and the electrochemical potential of each dot. Both single and double quantum dot configurations prove to be very stable and show excellent control over the electrostatic environment of the dots, making this system a highly versatile platform for spin-based quantum computing.
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