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Plasma etching has been a key driver of miniaturization technologies toward smaller and more powerful devices in the semiconductor industry. Thin layers involved in complex stacks of materials are approaching the atomic level. Furthermore, new categories of devices have complex architectures, leading to new challenges in terms of plasma etching. New plasma processes that are capable to etch ultra-thin layers of materials with control at the atomic level are now required. In this paper, the authors demonstrate that Si etching in Cl 2 plasma using plasma pulsing is a promising way to decrease the plasma-induced damage of materials. A controlled etch rate of 0.2 nm min− 1 is reported by pulsing the chlorine plasma at very low duty cycles. Using quasi-in-situ angle resolved XPS analyses, they show that the surface of crystalline silicon is less chlorinated, the amorphization of the top crystalline silicon surface is …