The vectorial control of magnetization by light

Application of coherent light–matter interactions has recently been extended to the ultrafast control of magnetization. An important but unrealized technique is the manipulation of magnetization vector motion to make it follow an arbitrarily designed multidimensional trajectory. Here we demonstrate a full manipulation of two-dimensional magnetic oscillations in antiferromagnetic NiO with a pair of polarization-twisted femtosecond laser pulses. We employ Raman-type nonlinear optical processes, wherein magnetic oscillations are impulsively induced with a controlled initial phase. Their azimuthal angle follows well-defined selection rules that have been determined by the symmetries of the materials. We emphasize that the temporal variation of the laser-pulse polarization angle enables us to control the phase and amplitude of the two degenerate modes, independently. These results lead to a new concept of the vectorial control of magnetization by light. Light–matter interactions can be used to manipulate magnetization in solids, but light-controlled magnetization vector motion has not been demonstrated. Here, two-dimensional magnetic oscillations in NiO are manipulated with optical pulses leading to vectorial control of magnetization by light.