Terahertz-Driven Nonlinear Spin Response of Antiferromagnetic Nickel Oxide

Terahertz magnetic fields with amplitudes of up to 0.4 Tesla drive magnon resonances in nickel oxide while the induced dynamics is recorded by femtosecond magneto-optical probing. We observe distinct spin-mediated optical nonlinearities, including oscillations at the second harmonic of the 1 THz magnon mode. The latter originate from coherent dynamics of the longitudinal component of the antiferromagnetic order parameter, which are probed by magneto-optical effects of second order in the spin deflection. These observations allow us to dynamically disentangle electronic from lattice-related contributions to magnetic linear birefringence and dichroism-information so far only accessible by ultrafast THz spin control. The nonlinearities discussed here foreshadow physics that will become essential in future subcycle spin switching.