High-harmonic spectroscopies reveal that fast energy transfer within 20 fs triggers ultrafast magnetic phase transition in Ni.

Heusler compounds are exciting materials for future spintronics applications because they display a wide range of tunable electronic and magnetic interactions. Here, we use a femtosecond laser to directly transfer spin polarization from one element to another in a half-metallic Heusler material, Co2MnGe. This spin transfer initiates as soon as light is incident on the material, demonstrating spatial transfer of angular momentum between neighboring atomic sites on time scales < 10 fs. Using ultrafast high harmonic pulses to simultaneously and independently probe the magnetic state of two elements during laser excitation, we find that the magnetization of Co is enhanced, while that of Mn rapidly quenches. Density functional theory calculations show that the optical excitation directly transfers spin from one magnetic sublattice to another through preferred spin-polarized excitation pathways. This direct manipulation of spins via light provides a path toward spintronic devices that can operate on few-femtosecond or faster time scales.

By correlating time- and angle-resolved photoemission and time-resolved transverse magneto-optical Kerr effect measurements, both at extreme ultraviolet wavelengths, we uncover the universal nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences-from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. Both probe methods exhibit the same demagnetization and recovery timescales. The spin system absorbs the energy required to proceed through a magnetic phase transition within 20 fs after the peak of the pump pulse. However, the spectroscopic signatures of demagnetization of the material appear only after ≈200  fs and the subsequent recovery of magnetization on timescales ranging from 500 fs to >70  ps. We also provide evidence of two competing channels with two distinct timescales in the recovery process that suggest the presence of coexisting phases in the material.

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The microscopic state of a magnetic material is characterized by its resonant magneto-optical response through the off-diagonal dielectric tensor component xy . However, the measurement of the full complex xy in the extreme ultraviolet spectral region covering the M absorption edges of 3d ferromagnets is challenging due to the need for either a careful polarization analysis, which is complicated by a lack of efficient polarization analyzers, or scanning the angle of incidence in fine steps. Here, we propose and demonstrate a new technique to extract the complex resonant permittivity xy simply by scanning the polarization angle of linearly polarized high harmonics to measure the magneto-optical asymmetry in reflection geometry. Because this technique is more practical and faster to experimentally implement than previous approaches, we can directly measure the full time evolution of xy (t) during laser-induced demagnetization across the entire M 2,3 absorption edge of cobalt with femtosecond time resolution. We find that for polycrystalline Co films on an insulating substrate, the changes in xy are uniform throughout the spectrum, to within our experimental precision. This result suggests that, in the regime of strong demagnetization, the ultrafast demagnetization response is primarily dominated by magnon generation. We estimate the contribution of exchange-splitting reduction to the ultrafast demagnetization process to be no more than 25%.