We demonstrate that optical pumping by circularly polarized light at the charge-transfer transition can induce spin and orbital polarizations in the strongly correlated Mott insulators R(2)CuO(4) (R=Pr, Nd, Sm) providing a means of ultrafast nonlinear manipulation of spin states on time scales of less than 150 fs. We propose a model which includes both orbital- and spin-related processes possessing different spectral and temporal properties. This allows us to model the optical response of antiferromagnetic Mott insulators to circularly polarized light and estimate the spin relaxation time as tau(s) approximately 30-50 fs.