Theory for the Nonlinear Optical Response of Transition-Metals: Polarization Dependence as a Fingerprint of the Electronic Structure at Surfaces and Interfaces

Surfaces and interfaces of magnetic nanostructures can reveal rather interesting and unusual properties that differ substantially from those of bulky materials. Here we apply the surface-sensitive method of optical second harmonic generation (SHG) for the studies of magnetization induced effects that appear in the nonlinear reflection from interfaces between ferromagnetic (Co) and heavy metals (Pt, Ta, W, Au, Ag, Cu). We demonstrate the appearance of magnetization induced var...

Nonlinear magneto-optics is a very sensitive fingerprint of the electronic, magnetic, and atomic structure of surfaces, interfaces, and thin ferromagnetic films. Analyzing theoretically the nonlinear magneto-optical Kerr effect for thin films of Fe(001) and at Fe surfaces we demonstrate exemplarily how various electronic material properties of ferromagnets , such as the $d$-band width, the magnetization, the substrate lattice constant, and the film-thickness dependence can be...

We extend our previous study of the polarization dependence of the nonlinear optical response to the case of magnetic surfaces and buried magnetic interfaces. We calculate for the longitudinal and polar configuration the nonlinear magneto-optical Kerr rotation angle. In particular, we show which tensor elements of the susceptibilities are involved in the enhancement of the Kerr rotation in nonlinear optics for different configurations and we demonstrate by a detailed analysis...

Using symmetry arguments we show how optical second harmonic generation (SHG) can be used to detect antiferromagnetism at surfaces and in thin films. Based on the group theoretical analysis of the nonlinear electric susceptibility we propose a new nonlinear magneto-optical effect, which allows even in the presence of unit-cell doubling for the unambiguous discri- mination of antiferromagnetic spin configurations from ferro- or paramagnetic ones. As an example for this effect ...

Spectroscopic magnetization induced optical Second Harmonic Generation (MSHG) measurements from a clean Ni(110) surface reveal strong resonance effects near 2.7 eV that can be attributed to the presence of an empty surface state. The good agreement with model calculations shows the potential of MSHG to probe spin polarized interface band structures.

Femtosecond pump-probe second-harmonic generation (SHG) and transient linear reflectivity measurements were carried out on polycrystalline Cu, Ag and Au in air to analyze whether the electron temperature affects Fresnel factors or nonlinear susceptibilities, or both. Sensitivity to electron temperatures was attained by using photon energies near the interband transition threshold. We find that the nonlinear susceptibility carries the electron temperature dependence in case of...

We compute the nonlinear optical response of an Fe monolayer placed on top of 1 to 4 monolayers of Cu(001). Our calculation is based on ab initio eigenstates of the slab, which are obtained within the full-potential linearized augmented plane-wave method. The ground-state spin-polarized electronic structure is converged self-consistently to an accuracy better than 0.1 mRy. Subsequently, we take the spin-orbit interaction into account within a second variational treatment. The...

We theoretically consider magnetization dynamics in a ferromagnetic slab induced by the magnetic field of a strong femtosecond laser pulse. The longitudinal geometry, in which the initial magnetization lies in both the plane of incidence and the sample plane, is studied. The magnetization oscillations at the optical wave frequency are calculated with the use of the Kapitza pendulum approach taking into account that the optical frequency is much greater than the magnetization ...

We experimentally explore the fingerprint of the microscopic electron dynamics in second-order harmonic generation (SHG). It is shown that the interbond electron hopping induces a novel source of nonlinear polarization and plays an important role even when the driving laser intensity is 2 orders of magnitude lower than the characteristic atomic field. Our model predicts anomalous anisotropic structures of the SHG yield contributed by the interbond electron hopping, which is i...

By uncovering novel aspects of second harmonic generation in aluminum we show that there are unusual and remarkable consequences of resonant absorption, namely an unexpectedly critical role that bound electrons play for light-matter interactions across the optical spectrum, suggesting that a different basic approach is required to fully explain the physics of surfaces. We tackle an issue that is never under consideration given the generic hostile conditions to the propagation...