Giant moment increase by ultrafast laser light

Abstract: It is now well established that a few femtosecond laser pulse will induce an ultrafast loss of moment in a magnetic material. Here we show that the opposite effect can also occur: an ultrafast increase in moment. Employing both tight-binding and state-of-the-art time dependent density functional theory we find that laser light tuned to the majority spin conduction band in the 2d magnets CrI$_3$ and CrSBr generates an ultrafast giant moment increase, of up to 33\% in the case of CrI$_3$ (2~$\mu_B$). Underpinning this is spin-orbit induced valence band spin texture that, in combination with a strong field light pulse, facilitates an optical spin flip transition involving both intra- and inter-band excitation. Our findings, that establish a general mechanism by which ultrafast light pulses may enhance as well as decrease the magnetic moment, point towards rich possibilities for light control over magnetic matter at femtosecond times.