Harmonic Generation from Metal-Oxide and Metal-Metal Boundaries

TL;DR

This paper investigates second- and third-harmonic generation at metal and metal-oxide boundaries, revealing how free-electron density discontinuities and epsilon-near-zero conditions influence nonlinear optical responses and can be engineered for enhanced harmonic emission.

Contribution

It introduces a microscopic hydrodynamic model to analyze harmonic generation at metal-oxide and metal-metal interfaces, emphasizing the role of free-electron density discontinuities and surface charge control.

Findings

Harmonic generation is sensitive to free-electron density discontinuities.

Epsilon-near-zero conditions enhance local fields and conversion efficiencies.

Surface charge engineering can control harmonic emission.

Abstract

We explore the outcomes of detailed microscopic models by calculating second- and third-harmonic generation from thin film surfaces with discontinuous free-electron densities. These circumstances can occur in structures consisting of a simple metal mirror, or arrangements composed of either different metals or a metal and a free electron system like a conducting oxide. Using a hydrodynamic approach we highlight the case of a gold mirror, and that of a two-layer system containing indium tin oxide (ITO) and gold. We assume the gold mirror surface is characterized by a free-electron cloud of varying density that spills into the vacuum, which as a result of material dispersion exhibits epsilon-near-zero conditions and local field enhancement at the surface. For a bylayer consisting of a thin ITO and gold films, if the wave is incident from the ITO side the electromagnetic field is presented with a free-electron discontinuity at the ITO/gold interface, and wavelength-dependent, epsilon-near-zero conditions that enhance local fields and conversion efficiencies, and determine the surface's emission properties. We evaluate the relative significance of additional nonlinear sources that arise when a free-electron discontinuity is present, and show that harmonic generation can be sensitive to the density of the screening free-electron cloud, and not its thickness. Our findings also suggest the possibility to control surface harmonic generation through surface charge engineering.