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The effect of electron confinement on the magnetocrystalline anisotropy of ultrathin bcc Fe films is explored by combining photoemission spectroscopy, x-ray magnetic circular dichroism, and magneto-optical Kerr effect measurements. Pronounced thickness-dependent variations in the magnetocrystalline anisotropy are ascribed to periodic changes in the density of states at the Fermi level, induced by quantization of ${d}_{xz}$, ${d}_{yz}$ out-of-plane orbitals. Our results reveal a direct correlation between quantum well states, the orbital magnetic moment, and the magnetocrystalline anisotropy.

In an interferometric pump-probe experiment, we demonstrate the phase tuning of the spin polarization of photoelectrons emitted in a three-photon process from Cu(001). A phase shift of pi between delayed ultrafast circularly polarized light pulses can switch the spin polarization from +/-20% to -/+40%. In the delay regime of overlapping pulses, we show the dominating role of optical interference effects in determining the spin polarization. For longer delays, we detect the influence of the coherent material response, manifested in both the final state electron population as well as the final state spin polarization.

We report the observation of a net spin polarization in the n=1 image-potential state at the Cu(001) surface. The spin polarization is achieved by spin-selective multiphoton excitation of electrons from the spin-orbit split Cu d bands to the image-potential state using circularly polarized ultrafast light pulses. We show that by tuning the exciting photon energy, we can adjust the resonant coupling of the image-potential state to d bands of different double-group symmetry. This allows us to tune the spin polarization injected into the image-potential state.

We observed high-order 2- to 4-photon photoemission and above threshold photoemission (ATP) processes with 3.07 eV light from the Cu(001) surface. The intensity of 3-photon photoemission via excitation through the $n=1$ image potential state significantly exceeded that of the 2-photon process. The ATP occurs either via single photon transitions from the image potential resonances above the vacuum level or by multiphoton transitions from image potential states below the vacuum level. The experimental ratio of the $m$- to $(m+1)$-photon process yields is sensitive to the electronic band structure of the solid.

We have investigated the possibility of isolating the step-induced in-plane uniaxial magnetic anisotropy in Fe/Ag(001) films on which nanoscale surface ripples were fabricated by the ion sculpting technique. For rippled Fe films deposited on flat Ag(001), the steps created along the ripple sidewalls are shown to be the only source of uniaxial anisotropy. Ion sculpting of ultrathin magnetic films allows one to selectively study the step-induced anisotropy and to investigate the correlation between local atomic environment and magnetic properties.

Magnetization-induced optical surface second harmonic generation (SHG) in the longitudinal geometry was used to study magnetism on the p(1 x 1)O/Fe(001) surface during a layer-by-layer Fe growth with surfactant oxygen. Considerable one-monolayer oscillations were observed. Minima of the magnetization-induced contributions to the second order dielectric susceptibility were detected at half-filled monolayers. These contributions were accessed either by measuring a purely magnetic SHG yield, or indirectly from the magnetization dependence of the overall SHG signal, both providing consistent results. The origin of the oscillatory surface magnetism is consistent with the expected oscillating oxygen induced relaxation due to the surface Fe islands.