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Register a new userRaman spectral shift versus strain and composition in GeSn layers with: 6 to 15% Sn contents
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GeSn alloys are the subject of intense research activities as these group IV semiconductors present direct bandgap behaviors for high Sn contents. Today, the control of strain becomes an important challenge to improve GeSn devices. Strain micro-measurements are usually performed by Raman spectroscopy. However, different relationships linking the Raman spectral shifts to the built-in strain can be found in the literature. They were deduced from studies on low Sn content GeSn layers (i.e. xSn<8%) or on GeSiSn layers. In this work, we have calibrated the GeSn Raman relationship for really high Sn content GeSn binaries (6<xSn<15%). We have used fully strained GeSn layers and fully relaxed GeSn under-etched microstructures to clearly differentiate the contributions of strain and chemical composition on the Ge-Ge Raman spectral shift. We have shown that the GeSn Raman-strain coefficient for high Sn contents is higher compared to that for pure Ge.
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We report on the behavior of Ge-Ge, Ge-Sn, Sn-Sn like and disorder-activated vibrational modes in GeSn semiconductors investigated using Raman scattering spectroscopy. By using an excitation wavelength close to E1 gap, all modes are clearly resolved and their evolution as a function of strain and Sn content is established. In order to decouple the individual contribution of content and strain, the analysis was conducted on series of pseudomorphic and relaxed epitaxial layers with a Sn content in the 5-17at.% range. All vibrational modes were found to display the same qualitative behavior as a function of content and strain, viz. a linear downshift as the Sn content increases or the compressive strain relaxes. Simultaneously, Ge-Sn and Ge-Ge peaks broaden, and the latter becomes increasingly asymmetric. This asymmetry, coupled with the peak position, is exploited in an empirical method to accurately quantify the Sn composition and lattice strain from Raman spectra.
GeSn epitaxial heterostructures are emerging as prominent candidates for the monolithic integration of light sources on Si substrates. Here we propose a judicious explanation for their temperature-dependent photoluminescence (PL) that is based upon the so far disregarded optical activity of dislocations. By working at the onset of plastic relaxation, which occurs whenever the epilayer releases the strain accumulated during growth on the lattice mismatched substrate, we demonstrate that dislocation nucleation can be explicitly seen in the PL data. Notably, our findings point out that a monotonous thermal PL quenching can be observed in coherent films, in spite of the indirect nature of the GeSn bandgap. Our investigation, therefore, contributes to a deeper understanding of the recombination dynamics in this intriguing group IV alloy and offers insights into crucial phenomena shaping the light emission efficiency.
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.
Raman spectroscopy is a powerful tool for characterizing the local properties of graphene. Here, we introduce a method for evaluating unknown strain configurations and simultaneous doping. It relies on separating the effects of hydrostatic strain (peak shift) and shear strain (peak splitting) on the Raman spectrum of graphene. The peak shifts from hydrostatic strain and doping are separated with a correlation analysis of the 2D and G frequencies. This enables us to obtain the local hydrostatic strain, shear strain and doping without any assumption on the strain configuration prior to the analysis. We demonstrate our approach for two model cases: Graphene under uniaxial stress on a PMMA substrate and graphene suspended on nanostructures that induce an unknown strain configuration. We measured $omega_mathrm{2D}/omega_mathrm{G} = 2.21 pm 0.05$ for pure hydrostatic strain. Raman scattering with circular corotating polarization is ideal for analyzing strain and doping, especially for weak strain when the peak splitting by shear strain cannot be resolved.
We report on the temperature stability of pseudomorphic GeSn films grown by molecular beam epitaxy on Ge(001) substrates. Both the growth temperature-dependence and the influence of post-growth annealing steps were investigated. In either case we observe that decomposition of metastable epilayers with Sn concentrations around 10% sets in above 230{deg}C, the eutectic temperature of the Ge/Sn system. Time-resolved annealing experiments in a scanning electron microscope reveal the crucial role of liquid Sn droplets in this phase separation process. Driven by a gradient of the chemical potential, the Sn droplets move on the surface along preferential crystallographic directions, thereby taking up Sn and Ge from the strained GeSn layer at their leading edge. While Sn-uptake increases the volume of the melt, dissolved Ge becomes re-deposited by a liquid-phase epitaxial process at the trailing edge of the droplet. Secondary droplets are launched from the rims of the single-crystalline Ge trails into intact regions of the GeSn film, leading to an avalanche-like transformation front between the GeSn film and re-deposited Ge. This process makes phase separation of metastable GeSn layers particularly efficient at rather low temperatures.
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