Non-Thermal Equilibrium Formation of Ge1-xSnx (0≤x≤0.2) Crystals on Insulator by Pulsed Laser Annealing

Abstract

Introduction Formation of crystalline GeSn film on insulator with high Sn concentration exceeding thermal equilibrium solid-solubility is strongly expected to realize high-speed thin film transistors. To explore non-thermal equilibrium processing [1], we examined crystallization of amorphous-GeSn (a-GeSn) with various modulated Sn concentration by pulsed laser annealing (PLA). In the present study, we focus on the influence of the Sn concentration on crystallization of a-GeSn by PLA. Experimental Procedure Schematic sample structure and PLA conditions are shown in Fig.1. A-Ge1-xSnx (0≦x≦0.2) films (thickness: 100 nm) were deposited on quartz substrates by a molecular beam technique. These samples were irradiated with a pulsed laser (energy : 10 - 230 mJ/cm2, pulse period : 1 sec, pulse number : 100 shot). The laser annealed regions were analyzed by Nomarski microscopy and Raman scattering spectroscopy. Results and Discussion Nomarski micrograph and Raman spectra of Ge0.8Sn0.2 samples before and after PLA with various energy are summarized in Fig. 2. In the samples after PLA, the contrast-changed regions were observed, compared with the as-deposited sample. Here, the contrast becomes stronger with increasing energy from 50 mJ/cm2 to 170 mJ/cm2, and finally the GeSn layer was damaged for energy of 230 mJ/cm2. Raman spectra reveales that Ge0.8Sn0.2 is crystallized on insulating substrates by 50 - 170 mJ/cm2 PLA. The process-window to achieve crystalline GeSn is summarized in Fig. 3(a), where the energy for starting crystallization and the energy just before damaging are indicated as Ecryst. and Edamage , respectively. Substitutional Sn concentration estimated from shift of Ge-Ge peak obtained by Raman measurements is shown in Fig. 3(b). The process window necessary for crystallization is significantly expanded by introducing Sn, i.e. 16 mJ/cm2 for Ge, ~ 130 mJ/cm2 for GeSn. High Sn concentration exceeding thermal equilibrium solid-solubility is obtained by PLA, for all GeSn samples. Interestingly, for samples with initial Sn concentration of 5 % and 10 %, almost all Sn atoms are incorporated into substitutional site, while for 20 % sample, only half of Sn atoms are incorporated into substitutional site. The detailed physics will be discussed in the presentation.