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We present a scalable technology at room temperature for the fabrication of ultrathin films based on surfactant-free surface-engineered silicon nanocrystals (SiNCs). Environmentally friendly pulsed fsec laser induced surface engineering of SiNCs and vacuum low-angle spray deposition is used to produce ultrathin films. Surface engineering of SiNCs improved stability and dispersibility of SiNCs by allowing thin (30 nm thickness) and exceptionally smooth (mean square roughness corresponds to 0.32doi:10.1002/ese3.165 fatcat:fju2ndvo6rewvj24ux5y2lks64