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

Plasmonic resonances in metallic nanostructures have been shown to drastically enhance local electromagnetic fields, and thereby increase the efficiency of nonlinear optical phenomena, such as second harmonic generation (SHG). While it has been experimentally observed that enhanced fields can significantly boost SHG, to date it proved difficult to probe electrical and magnetic resonances in one and the same nanostructure. This however is necessary to directly compare relative...

Optical second harmonic generation is a second-order nonlinear process that combines two photons of a given frequency into a third photon at twice the frequency. Due to the symmetry constraints, it is widely used as a sensitive probe to detect broken inversion symmetry and local polar order. Analytical modeling of the electric-dipole SHG response is essential to extract fundamental properties of materials from experiments. However, complexity builds up dramatically in the ana...

Using group theory we classify the nonlinear magneto-optical response at low-index surfaces of fcc antiferromagnets, such as NiO. Structures consisting of one atomic layer are discussed in detail. We find that optical second harmonic generation is sensitive to surface antiferromagnetism in many cases. We discuss the influence of a second type of magnetic atoms, and also of a possible oxygen sublattice distortion on the output signal. Finally, our symmetry analysis yields the ...

Second-order nonlinear optical processes do not manifest in the bulk of centrosymmetric materials, but may occur in the angstroms-thick layer at surfaces. At such length-scales, quantum mechanical effects come into play which could be crucial for an accurate description of plasmonic systems. In this article, we develop a theoretical model based on the quantum hydrodynamic description to study free-electron nonlinear dynamics in plasmonic systems. Our model predicts strong res...

We present a modeling of the nonlinear optical response of a metal surface in order to account for recent experimental results from two-color Sum-Frequency Generation experiments on gold. The model allows calculating the surface and bulk contributions, and explicitly separates free and bound electron terms. Contrary to the other contributions, the perpendicular surface component is strongly model-dependent through the surface electron density profiles. We consider three elect...

We present a study of the second-order nonlinear optical properties of metal-based metamaterials. A hydrodynamic model for electronic response is used, in which nonlinear surface contributions are expressed in terms of the bulk polarization. The model is in good agreement with published experimental results, and clarifies the mechanisms contributing to the nonlinear response. In particular, we show that the reported enhancement of second-harmonic in split-ring resonator based...

The study of the non-linear response of matter to high electric fields has recently encompassed harmonic generation in solids at near-infrared (NIR) driving wavelengths. Interest has been driven by the prospect of ultrafast signal processing and all-optical mapping of electron wave-functions in solids. Engineering solid-state band structures to control the non-linear process has already been highlighted theoretically. Here, we show experimentally for the first time that secon...

Nonlinear optical frequency conversion, where optical fields interact with a nonlinear medium to generate new frequencies, is a key phenomenon in modern photonic systems. However, a major challenge with these techniques lies in the difficulty of tuning the nonlinear electrical susceptibilities that drive such effects in a given material. As a result, dynamic control of optical nonlinearities has remained largely confined to research laboratories, limiting its practical use as...

Extending our previous work we classify the nonlinear magneto-optical response at low index surfaces of fcc antiferromagnets, such as NiO. Antiferromagnetic bilayers are discussed here as models for the termination of bulk antiferromagnets.

NiO is a good candidate for ultrafast magnetic switching because of its large spin density, antiferromagnetic order, and clearly separated intragap states. In order to detect and monitor the switching dynamics, we develop a systematic approach to study optical second harmonic generation (SHG) in NiO, both at the (001) surface and in the bulk. In our calculations NiO is modeled as a doubly embedded cluster. All intragap \emph{d}-states of the bulk and the (001) surface are obt...