Tunable second harmonic generation in 2D materials: comparison of different strategies

TL;DR

This paper investigates methods to electrically tune second harmonic generation in 2D materials, comparing two configurations through ab-initio simulations to enable dynamic control of nonlinear optical responses.

Contribution

It introduces and compares two strategies for electrically manipulating second-order nonlinearity in 2D materials using real-time ab-initio methods.

Findings

External fields can induce SHG in non-SHG materials.

Doping alters the intensity of existing SHG signals.

Comparison with experiments highlights method limitations.

Abstract

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 a spectroscopic tool. In this work, we aim to advance the development of devices with tunable nonlinear responses by exploring two potential mechanisms for electrically manipulating second-order optical nonlinearity in two-dimensional materials. Specifically, we consider two configurations: in the first, the material does not inherently exhibit second-harmonic generation (SHG), but this response is induced by an external field; in the second, an external field induces doping in a material that already exhibits SHG, altering the intensity of the nonlinear signal. In this work, we have studied these two configurations using a real-time ab-initio approach under an out-of-plane external field and including the effects of doping-induced variations in the screened electron-electron interaction. We then discuss the limitations of current computational methods and compare our results with experimental measurements.