نبذة مختصرة : This paper presents a new approach for material removal on silicon at atomic and close-to-atomic scale assisted by photons. The corresponding mechanisms are also investigated. The proposed approach consists of two sequential steps: surface modification and photon irradiation. The back bonds of silicon atoms are first weakened by the chemisorption of chlorine and then broken by photon energy, leading to the desorption of chlorinated silicon. The mechanisms of photon-induced desorption of chlorinated silicon, i.e., SiCl2 and SiCl, are explained by two models: the Menzel–Gomer–Redhead (MGR) and Antoniewicz models. The desorption probability associated with the two models is numerically calculated by solving the Liouville–von Neumann equations for open quantum systems. The calculation accuracy is verified by comparison with the results in literatures in the case of the NO/Pt (111) system. The calculation method is then applied to the cases of SiCl2/Si and SiCl/Si systems. The results show that the value of desorption probability first increases dramatically and then saturates to a stable value within hundreds of femtoseconds after excitation. The desorption probability shows a super-linear dependence on the lifetime of excited states.
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