Employing spin-, time-, and energy-resolved photoemission spectroscopy, we present the first study on the spin polarization of a single electronic state after ultrafast optical excitation. Our investigation concentrates on the majority-spin component of the d-band-derived Gd(0001) surface state d(z(2))(↑). While its binding energy shows a rapid Stoner-like shift by 90 meV with an exponential time constant of τ(E)=0.6±0.1 ps, the d(z(2))(↑) spin polarization remains nearly constant within the first picoseconds and decays with τ(S)=15±8  ps. This behavior is in clear contrast to the equilibrium phase transition, where the spin polarization vanishes at the Curie temperature.

For the generation of spin-polarized photocurrents in topological insulators, a coupling between photon angular momentum and electron spin is often assumed. Such a coupling seems to be supported by dichroism reported in E(k y)-intensity maps in photoemission. We show in three dimensional two-photon photoemission and one-step photoemission calculations that the circular dichroism is in fact threefold in E(k x , k y) maps although it may appear antisymmetric in E(k y). The threefold symmetry is inconsistent with the previously assumed coupling between photon momentum and electron's chiral spin via the orbital momentum. Instead it reflects the surface point group. The only antisymmetric patterns appear in the energy range in which surface and bulk states hybridize. In general, a threefold-symmetric dichroic signal does not support unidirectional photocurrents. Nevertheless, the residual asymmetry of up to 3.5% in our photoemission spectra is compatible with previously observed helicity-dependent photocurrents.

We report on a spin-resolved two-photon photoemission study of the Ni(1 1 1) surface states. Nickel thin films were grown by molecular beam epitaxy on a W(1 1 0) substrate. The first image-potential state is used as a sensor to map the spin polarization of the occupied surface states. This allows us to identify the majority spin component of the Shockley surface state as well as a majority and minority d-derived surface resonance. The n = 1 image-potential state is found to be exchange split by 14 ± 3 meV. In spite of the fact that the band structure at the Fermi level exhibits a strongly discerned density of states in both spin channels, we observe low spin asymmetries in the decay and dephasing rates of the photoexcited electrons. Varying the sample preparation reveals that the Shockley surface state contributes about 40% to the spin-dependent decay rate.

By comparing femtosecond laser-pulse-induced spin dynamics in the surface state of the rare earth metals Gd and Tb, we show that the spin polarization of valence states in both materials decays with significantly different time constants of 15 ps and 400 fs, respectively. The distinct spin polarization dynamics in Gd and Tb are opposed by similar exchange splitting dynamics in the two materials. The different time scales observed in our experiment can be attributed to weak and strong 4f spin to lattice coupling in Gd and Tb, suggesting an intimate coupling of spin polarization and 4f magnetic moment. While in Gd the lattice mainly acts as a heat sink, it contributes significantly to ultrafast demagnetization of Tb. This helps explain why all optical switching is observed in FeGd—but rarely in FeTb-based compounds.

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