Light-driven Electrodynamics and Demagnetization in FenGeTe2 (n = 3, 5) Thin Films

Abstract Two-dimensional materials-based ultrafast spintronics is expected to surpass conventional data storage and manipulation technologies, that are now reaching their fundamental limits. The newly discovered van der Waals (VdW) magnets provide a new platform for ultrafast spintronics since their magnetic and electrical properties can be tuned by many external factors, such as strain, voltage, magnetic field, or light absorption for instance. Here, we report on the direct relationship between magnetic order and Terahertz (THz) electrodynamics in FenGeTe2 (n = 3, 5) (FGT) films after being illuminated by a femtosecond optical pulse, studying their ultrafast THz response as a function of the optical pump-THz probe temporal delay. In Fe5GeTe2, we find clear evidence that light-induced electronic excitations directly influence THz electrodynamics similarly to a demagnetization process, contrasting with the effects observed in Fe3GeTe2, which are characterized by a thermal energy transfer among electrons, magnons, and phonons. We address these effects as a function of the pump fluence and pump-probe delay, and by tuning the temperature across the magnetic ordering Curie temperature, highlighting the microscopic mechanisms describing the out-of-equilibrium evolution of the THz conductivity. Finally, we find evidence for the incoherent-coherent crossover predicted by the Kondo-Ising scenario in Fe3GeTe2 and successfully simulate its light-driven electrodynamics through a three-temperature model. As indicated by these results, FGT surpasses conventional metals in terms of modulating its properties using an optical lever.