advance the present, fully group-IV-based room temperature light-emitting devices [6] or photodetectors. [7,8] For many of these applications, the Ge concentrations x for the thick but pseudomorphic Si 1-x Ge x films (TPFs) should be ideally in the range between 50% and 100%, to ensure, e.g., large enough band offsets between the Si and SiGe layers. [5,9] However, the literature reports mainly focus on TPFs with low Ge contents, x < 0.5, [10][11][12][13][14][15][16][17][18] with only a few exceptions for which the critical thickness for pronounced relaxation was evaluated for single Ge concentrations of about 55%. [11,17] In general, during the growth of strained epitaxial layers, the strain energy increases with the square of the misfit strain and linearly with the layer thickness. Thus, TPFs must release the inherent strain energy by either plastic or elastic relaxation above a misfit strain-dependent critical thickness (t c ). The former via the insertion of misfit dislocations, [19] the latter via an increase in surface energy, i.e., by forming 3D objects, such as surface undulations, quantum dots, or wires. [20] A general trend confirmed by this work is that for sufficiently high growth temperatures and beyond t c for flat film growth, lower misfits lead to the formation of dislocations (plastic relaxation), while for high misfits, typically 3D nanostructures form via elastic relaxation. [12,21,22] Along similar lines, a mixture of low-and high-temperature growth can be used to produce flat relaxed films, starting from low-temperature growth to favor dislocation insertion, followed by high-temperature growth to increase the film quality. [23][24][25] Equilibrium theory for t c of TPFs was first developed in the 70s [26,27] but did not consider that, in reality, the growth of TPFs, e.g., by molecular beam epitaxy (MBE), happens far from thermal equilibrium. Hence, the kinetic suppression of either dislocation nucleation or quantum dot formation at low growth temperatures (T G ) explains why for Ge concentrations x < 55% experimentally found values of t c exceed those predicted by equilibrium theory by about an order of magnitude. [11,17,[28][29][30] Along the same lines, it was shown that supersaturation in the wetting layer (WL) occurs before the nucleation of quantum dots or wires during the epitaxial deposition of pure Ge thin films. [31] However, at T G ¼ 700 °C, the supersaturation amounts to only %0.14 nm of Ge, and quantum dot formation occurs already after the deposition of 0.6 nm. [32] Notably, the onset of quantum dot formation can be accelerated or delayed by increasing or decreasing T G , respectively. [33,34]