It is well established that light can control magnetism in matter, e.g. via the inverse Faraday effect or ultrafast demagnetization. However, such control is typically limited to magnetization transverse to light’s polarization plane or out-of-plane magnetism in two-dimensional (2D) materials, while in-plane magnetic moments have remained largely unexplored. This is due to the difficulty of generating electronic orbital angular momentum components within light’s polarization plane. Here we overcome this limitation, demonstrating complete three-dimensional all-optical control of magnetism in 2D materials. Using first-principles simulations, we show that a tailored two-color laser field can induce and steer magnetic moments in any direction with the relative angle between the laser polarizations playing a key parameter in coherent control. We analyze the physical mechanism of this process and show that it arises from a simultaneous breaking of time-reversal and spatial-inversion symmetries in the two-color laser. In-plane orbital moments are introduced via nonzero out-of-plane longitudinal photogalvanic currents enabled by broken-inversion and mirror symmetries, while time-reversal symmetry breaking enables buildup of spin-flip and rotation processes through spin-orbit coupling, translating the orbital moments to transient magnetism. Our findings demonstrate a full 3D coherent control scheme for transient magnetic states on femtosecond timescales driven by tailored lasers, and can be used to develop novel spectroscopies for magnetism, all-optical magnetic switching for ultrafast spintronics, and novel information storage capabilities.

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• Light-induced magnetic effects
• Nonlinear optics
• Photogalvanic effect
• Ultrafast magnetic effects
• 2-dimensional systems
• Time-dependent DFT