Ultrafast spin transfer and its impact on the electronic structure.

Optically induced intersite spin transfer (OISTR) promises manipulation of spin systems within the ultimate time limit of laser excitation. Following its prediction, signatures of ultrafast spin transfer between oppositely aligned spin sublattices have been observed in magnetic alloys and multilayers. However, it is known neither from theory nor from experiment whether the band structure immediately follows the ultrafast change in spin polarization or whether the exchange split bands remain rigid. We show that ultrafast spin transfer occurs even in ferromagnetic gadolinium metal. Charge transfer between localized surface and extended valence-band states leads to a decrease of the surface spin polarization. This synchronously alters the exchange splitting of the bulk valence bands during laser excitation. Moreover, the onset of demagnetization can be tuned by over 200 fs by changing the temperature-dependent spin mixing. Our results show a promising route to ultrafast control of the magnetization, widening the impact and applicability of OISTR.

Separating Exchange Splitting from Spin Mixing in Gadolinium by Femtosecond Laser Excitation.

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.

Spin-dependent lifetime and exchange splitting of surface states on Ni(1 1 1).

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.