Investigation of GeSn Strain Relaxation and Spontaneous Composition Gradient for Low-Defect and High-Sn Alloy Growth

Recent development of group-IV alloy GeSn indicates its bright future for the application of mid-infrared Si photonics. Relaxed GeSn with high material quality and high Sn composition is highly desirable to cover mid-infrared wavelength. However, its crystal growth remains a great challenge. In this work, a systematic study of GeSn strain relaxation mechanism and its effects on Sn incorporation during the material growth via chemical vapor deposition was conducted. It was discovered that Sn incorporation into Ge lattice sites is limited by high compressive strain rather than historically acknowledged chemical reaction dynamics, which was also confirmed by Gibbs free energy calculation. In-depth material characterizations revealed that: (i) the generation of dislocations at Ge/GeSn interface eases the compressive strain, which offers a favorably increased Sn incorporation; (ii) the formation of dislocation loop near Ge/GeSn interface effectively localizes defects, leading to the subsequent low-defect grown GeSn. Following the discovered growth mechanism, a world-record Sn content of 22.3% was achieved. The experiment result shows that even higher Sn content could be obtained if further continuous growth with the same recipe is conducted. This report offers an essential guidance for the growth of high quality high Sn composition GeSn for future GeSn based optoelectronics.