The magnetic cooling effect originates from a large change in entropy by the forced magnetization alignment, which has long been considered to be utilized as an alternative environment-friendly cooling technology compared to conventional refrigeration. However, an ultimate timescale of the magnetic cooling effect has never been studied yet. Here, we report that a giant magnetic cooling (up to 200 K) phenomenon exists in the Co/Pt nano-multilayers on a femtosecond timescale during the photoinduced demagnetization and remagnetization, where the disordered spins are more rapidly aligned, and thus magnetically cooled, by the external magnetic field via the lattice-spin interaction in the multilayer system. These findings were obtained by the extensive analysis of time-resolved magneto-optical responses with systematic variation of laser fluence as well as external field strength and direction. Ultrafast giant magnetic cooling observed in the present study can enable a new avenue to the realization of ultrafast magnetic devices.

Time‐resolved magneto‐optical Kerr effect measurement is carried out to determine ultrafast hysteresis behavior during a photo‐induced demagnetization/remagnetization process for Co/Pt ferromagnetic multilayers. Due to the stroboscopic measurement scheme, hysteresis curve measured by a pump–probe technique exhibits an irreversible behavior, repeatedly reset to a metastable hysteresis state at each stroboscopic measurement, observed as the reduction of the coercivity. It is demonstrated that the stroboscopically measured hysteresis and the coercivity could be a stable parameter in describing the ultrafast photo‐induced spin dynamics for both reversible and irreversible behaviors. Moreover, it is found that an unusual coercivity behavior exists together with a nontrivial magnetization change under external fields comparable to the coercivity of the sample.