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

A unified response theory for the time-resolved nonlinear light generation and two-photon photoemission (2PPE) from metal surfaces is presented. The theory allows to describe the dependence of the nonlinear optical response and the photoelectron yield, respectively, on the time dependence of the exciting light field. Quantum-mechanical interference effects affect the results significantly. Contributions to 2PPE due to the optical nonlinearity of the surface region are derived...

Metallic structures interacting with electromagnetic fields are known to exhibit properties similar to those found in atoms and molecules, such as multi-photon and tunnel ionization. Developing this similarity beyond the electron emission current, we generalize the wellknown Fowler-Nordheim model, and predict heretofore unrecognized source of nonlinear optical response from nano-structures exposed to illumination with intense optical pulses.

Complex oxide heterointerfaces and van der Waals heterostructures present two versatile but intrinsically different platforms for exploring emergent quantum phenomena and designing new functionalities. The rich opportunity offered by the synergy between these two classes of materials, however, is yet to be charted. Here, we report an unconventional nonlinear optical filtering effect resulting from the interfacial polar alignment between monolayer MoS$_2$ and a neighboring fer...

Spectroscopy of magnetization-induced second-harmonic generation (MSHG) is studied in magnetic Co$_{x}$Ag$_{1-x}$ granular films containing Co nanoparticles. A strong resonance of the magnetic contrast of the second-harmonic generation (SHG) intensity is observed in the two-photon energy range from 3,8 eV to 4,5 eV. The local surface plasmons exited in magnetic Co nanogranules in this spectral range assist MSHG and are responsible for a significant enhancement of the SHG magn...

The nonlinear magneto-optical response of $s$- and $d$-wave superconductors is discussed. We carry out the symmetry analysis of the nonlinear magneto-optical susceptibility in the superconducting state. Due to the surface sensitivity of the nonlinear optical response for systems with bulk inversion symmetry, we perform a group theoretical classification of the superconducting order parameter close to a surface. For the first time, the mixing of singlet and triplet pairing sta...

We experimentally study the optical second harmonic generation (SHG) from deep subwavelength gold-silver heterodimer and silver-silver and gold-gold homodimers. Our results show that the SHG from the heterodimer is about an order of magnitude more intense. In contrast, calculations based on known theory suggest that it is the silver-silver homodimer that should have the upper hand, putting the present theoretical view at odds with our experimental findings. Following this obs...

We analyze laser-induced ultrafast, spatially inhomogeneous magnetization dynamics of epitaxial Co/Cu(001) films in a 0.4-10 nm thickness range with time-resolved magnetization-induced second harmonic generation, which probes femtosecond spin dynamics at the vacuum/Co and Co/Cu interfaces. The interference of these two contributions makes the overall signal particularly sensitive to differences in the transient magnetization redistribution between the two interfaces, i.e. ult...

Near-infrared-to-visible second harmonic generation from air-stable two-dimensional polar gallium and indium metals is described. The photonic properties of 2D metals - including the largest second-order susceptibilities reported for metals (approaching 10nm$^2$/V) - are determined by the atomic-level structure and bonding of two-to-three-atom-thick crystalline films. The bond character evolved from covalent to metallic over a few atomic layers, changing the out-of-plane meta...

We show that, under the effect of an external magnetic field, a photogalvanic effect and the generation of second harmonic wave can be induced in inversion-symmetric and time reversal invariant Dirac semimetals. The mechanism responsible of these non linear optical responses is the magnetochiral effect. The origin of this magnetochiral effect is the band bending of the dispersion relation in real Dirac semimetals. Some observable consequences of this phenomenon are the appear...

Using density functional theory calculations, we have found an enhanced magneto-optical Kerr effect in Fe/insulator interfaces. The results of our study indicate that interfacial Fe atoms in the Fe films have a low-dimensional nature, which causes the following two effects: (i) The diagonal component $\sigma_{xx}$ of the optical conductivity decreases dramatically because the hopping integral for electrons between Fe atoms is suppressed by the low dimensionality. (ii) The off...