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Ultrathin single crystal Si films offer a versatile vehicle for high performance flexible and semitransparent electric devices due to their outstanding optoelectric and mechanical properties. Here, we demonstrate the formation of an ultrathin (100) single crystal Si film based on morphological evolution of nanoporous Si during high temperature annealing. Square arrays of cylindrical Si pores are formed by nanoimprint lithography and deep reactive etching and then subjected to annealing in hydrogen ambient. By controlling the aspect ratio of nanoporous Si, defect-free single crystal Si membranes with controlled thicknesses from 330 to 470 nm are formed on a platelike void after the annealing. In addition, we investigate the role of oxygen impurities in a hydrogen atmosphere on defect formation on a Si surface and eliminate the oxygen-related defects on Si by controlling gas phase diffusion of oxygen impurities during …