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We report about the dephasing of the spins states in a Garnet film excited byfemtosecond laser pulses. It is shown that magneto-optical four-wave-mixingsignals are efficiently generated and controlled with an external staticmagnetic field. The self-diffraction of either two or three femtosecond pulsesallows us determining independently the coherent response time ($T_2$ < 50 fs)and the population relaxation, which occurs in several steps. After the laserinduced demagnetization, the spin-lattice relaxation is the dominant mechanism($T_{1,spin-lat}$ < 1.35 ps) and the precession of the magnetization takesplace at later times ($T_{1,prec}$ < 150 ps). The coherent response of thespins states is modeled with a multi-level hydrogen-like system, taking intoaccount the fundamental relativistic quantum dynamics of the spins. Ourexperimental approach is general and opens the way to investigating quantummagnetism in ordered magnetic systems useful for applications in informationand communications technologies.

Coherent Magnetism and Spin-Orbit Interaction in Garnet Films Probed with Femtosecond Magneto-Optical Four Wave Mixing