First-principles calculations are used to investigate the structure, electronic and optical properties of silicon nanocystals with chlorine-passivated surface. The nanocrystals considered were approximately spherical, with diameters between 1.5 and 3.0 nm. We show that the nanocrystals with chlorinated surface have a smaller bandgap, lower optical absorption threshold, and greater ionization energy and electron affinity than hydrogenated silicon nanocrystals of the same size