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The ability to manipulate the composition of semiconductor alloys on demand and at nanometer-scale resolutions is a powerful tool that could be exploited to tune key properties such as the electronic band gap, mobility, and refractive index. However, existing methods to modify the composition involve altering the stoichiometry by temporal or spatial modulation of the process parameters during material growth, limiting the scalability and flexibility for device fabrication. Here, we report a laser processing method for localized tailoring of the composition in amorphous silicon-germanium (a-SiGe) nanoscale thin films on silicon substrates, postdeposition, by controlling phase segregation through the scan speed of the laser-induced molten zone. Laser-driven phase segregation at speeds adjustable from 0.1 to 100 mm s -1 allows access to previously unexplored solidification dynamics. The steady-state spatial distribution of the alloy constituents can be tuned directly by setting the laser scan speed constant to achieve indefinitely long Si 1- x  Ge  x  microstructures, exhibiting the full range of compositions (0 &lt; x &lt; 1). To illustrate the potential, we demonstrate a photodetection application by exploiting the laser-written polycrystalline SiGe microstripes, showing tunability of the optical absorption edge over a wavelength range of 200 nm. Our method can be applied to pseudobinary alloys of ternary semiconductors, metals, ceramics, and organic crystals, which have phase diagrams similar to those of SiGe alloys. This study opens a route for direct laser writing of novel devices made of alloy microstructures with tunable composition profiles, including graded-index waveguides and metasurfaces, multispectral photodetectors, full-spectrum solar cells, and lateral heterostructures.

Laser-Driven Phase Segregation and Tailoring of Compositionally Graded Microstructures in Si–Ge Nanoscale Thin Films