Two-colour surface optical rectification: Route to all-optical control of terahertz emission from quasi-2D structures

Nonlinear optics in sub-wavelength structures plays a crucial role in the development of integrated photonics platforms and devices [1]. Surfaces, nanostructures and two-dimensional media are inherently free from longitudinal phase matching constraints and constitute an attractive framework to engineer complex forms of lightmatter interactions [2-3]. Most recent efforts in this area have focused on the generation of frequencies in the optical and infrared regions, e.g., second or third harmonic generation. An open question, however, is whether the broadband frequency conversion enabled by nanoscale nonlinear media could lead to the generation of long-wavelength radiation in a process known as Optical Rectification (OR). To date, OR of ultrafast optical pulses in nonlinear media has been subject of intense research, since it provides a robust and versatile approach to generate and manipulate broadband Terahertz (THz) fields. Using non-centrosymmetric crystals such as ZnTe and LiNbO3, large bandwidth THz pulses limited mainly by longitudinal phase-matching constraints, could be achieved [4]. Highly nonlinear Quasi-2D structures represent an intriguing alternative to this popular approach.