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We propose Raman-induced collinear difference-frequency generation (DFG) as amethod to manipulate dynamical magnetization. When a fundamental beampropagates along a threefold rotational axis, this coherent second-orderoptical process is permitted by angular momentum conservation through therotational analogue of the Umklapp process. As a demonstration, weexperimentally obtained polarization properties of collinear magnetic DFG alonga [111] axis of a single crystal of antiferromagnetic NiO with micromultidomain structure, which excellently agreed with the theoreticalprediction.

Optical control of magnetization of micron-size domains in antiferromagnetic NiO single crystals