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

The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.

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.

We propose a sub-Doppler laser cooling mechanism that takes advantage of the unique spectral features and extreme dispersion generated by the phenomenon of electromagnetically induced transparency (EIT). EIT is a destructive quantum interference phenomenon experienced by atoms with multiple internal quantum states when illuminated by laser fields with appropriate frequencies. By detuning the lasers slightly from the "dark resonance", we observe that, within the transparency window, atoms can be subject to a strong viscous force, while being only slightly heated by the diffusion caused by spontaneous photon scattering. In contrast to other laser cooling schemes, such as polarization gradient cooling or EIT-sideband cooling, no external magnetic field or strong external confining potential is required. Using a semiclassical approximation, we derive analytically quantitative expressions for the steady-state temperature, which is confirmed by full quantum mechanical numerical simulations. We find that the lowest achievable temperatures approach the single-photon recoil energy. In addition to dissipative forces, the atoms are subject to a stationary conservative potential, leading to the possibility of spatial confinement. We find that under typical experimental parameters this effect is weak and stable trapping is not possible.