Peculiarities and evolution of Raman spectra of multilayer Ge/Si(001) heterostructures containing arrays of low‐temperature MBE‐grown Ge quantum dots of different size and number density: Experimental studies and numerical simulations

Ge/Si(001) multilayer heterostructures containing arrays of low‐temperature self‐assembled Ge quantum dots and very thin SixGe1−x layers of varying composition and complex geometry have been studied using Raman spectroscopy and scanning tunneling microscopy (STM). The dependence of Raman spectra on the effective thickness of deposited Ge layers has been investigated in detail in the range from 4 to 18 Å. The position and shape of both Ge and SiGe vibrational modes are of great interest because they are closely related to the strain and composition of the material that plays a role of active component in perspective optoelectronic devices based on such structures. In this work, we present an explanation for some peculiar features of Raman spectra, which makes it possible to control the quality of the grown heterostructures more effectively. A dramatic increase of intensity of both the Ge–Ge and Si–Ge bands for the structure containing Ge layers of 10 Å and anomalous shift and broadening of the Si–Ge band for structures comprising Ge layers of 8 and 9 Å thick were observed. In our model, the anomalous behavior of the Raman spectra with the change of thickness of deposited Ge is connected with the flatness of Ge layers as well as transitional SiGe domains formed via the stress‐induced diffusion from {105} facets of quantum dots. The conclusions are supported by the STM studies and the numerical calculations. The unique features of Raman spectra obtained from Ge/Si heterostructures containing Ge quantum dots were revealed and explained in terms of the changes in morphology of a Ge layer during its growth and further covering by Si. The mechanism of stress‐induced diffusion from facets of quantum dots leading to the forming of a transition SiGe layer is described. The suggested model is supported by numerical simulation of Raman spectra.