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We demonstrate the laser mediated atomic layer etching (ALEt) of silicon. Using a nanosecond pulsed 266 nm laser focused loosely over and in a parallel configuration to the surface of the silicon, we dissociate Cl2 gas to induce chlorination. Then, we use pulsed picosecond irradiation to remove the chlorinated layer. Subsequently, we perform continuous wave (CW) laser annealing to eliminate amorphization caused by the picosecond laser etching. Based on atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS), we observed strong evidence of chlorination and digital etching at 0.85 nm etching per cycle with good uniformity. 

Chemical doping can be used to control the charge-carrier polarity and concentration in two-dimensional van der Waals materials. However, conventional methods based on substitutional doping or surface functionalization result in the degradation of electrical mobility due to structural disorder, and the maximum doping density is set by the solubility limit of dopants. Here we show that a reversible laser-assisted chlorination process can be used to create high doping concentrations (above 3 × 1013 cm−2) in graphene monolayers with minimal drops in mobility. The approach uses two lasers—with distinct photon energies and geometric configurations—that are designed for chlorination and subsequent chlorine removal, allowing highly doped patterns to be written and erased without damaging the graphene. To illustrate the capabilities of our approach, we use it to create rewritable photoactive junctions for graphene-based photodetectors. 

Both amorphous and crystalline silicon are ubiquitous materials for electronics, photonics, and microelectromechanical systems. On‐demand control of Si crystallinity is crucial for device manufacturing and to overcome the limitations of current phase‐change materials (PCM) in active photonics. Fast reversible phase transformation in silicon, however, has never been accomplished due to the notorious challenge of amorphization. It is demonstrated that nanostructured Si can function as a PCM, since it can be reversibly crystallized and amorphized under nanosecond laser irradiation with different pulse energies. Reflection probing on a single nanodisk's phase transformations confirms the distinct mechanisms for crystallization and amorphization. The experimental results show that the relaxation time of undercooled silicon at 950 K is 10 ns. The phase change provides a 20% nonvolatile reflectivity modulation within 100 ns and can be repeated over 400 times. It is shown that such transformations are free of deformation upon solidification. Based on the switchable photonic properties in the visible spectrum, proof‐of‐concept experiments of dielectric color displays and dynamic wavefront control are shown. Therefore, nanostructured silicon is proposed as a chemically stable, deformation free, and complementary metal–oxide‐semiconductor compatible (CMOS) PCM for active photonics at visible wavelengths.