We demonstrate monolithic aluminum gallium arsenide (AlGaAs) optical anoantennas.Using a selective oxidation technique, we fabricate such epitaxial semiconductor nanoparticles on an aluminum oxide substrate. Second harmonic generation from an AlGaAs nanocylinder of height h=400 nm and varying radius pumped with femtosecond pulses delivered at 1554-nm wavelength has been measured, revealing a peak conversion efficiency exceeding 10 -5 for nanocylinders with an otpimized geometry.

We demonstrate that a dielectric anapole resonator on a metallic mirror can enhance the third harmonic emission by two orders of magnitude compared to a typical anapole resonator on an insulator substrate. By employing a gold mirror under a silicon nanodisk, we introduce a novel characteristic of the anapole mode through the spatial overlap of resonantly excited Cartesian electric and toroidal dipole modes. This is a remarkable improvement on the early demonstrations of the anapole mode in which the electric and toroidal modes interfere off-resonantly. Therefore, our system produces a significant near-field enhancement, facilitating the nonlinear process. Moreover, the mirror surface boosts the nonlinear emission via the free-charge oscillations within the interface, equivalent to producing a mirror image of the nonlinear source and the pump beneath the interface. We found that these improvements result in an extremely high experimentally obtained efficiency of 0.01%.

We review recent achievements in the field of nanoscale nonlinear AlGaAs photonics based on all-dielectric optical antennas. After discussing the motivation and main technological challenges for the development of an AlGaAs monolithic platform for χ nonlinear nanophotonics, we present numerical and experimental investigations of the second-order nonlinear response and physical reasons for high efficiency of second-order nonlinear interactions in the AlGaAs nano-antennas. In particular, we emphasize the role of the dipolar resonances at the fundamental frequency and the multipolar resonances at the second harmonic wavelength. We also discuss second-harmonic generation directionality and show possible strategies to engineer the radiation pattern of nonlinear antennas.

Monolayer transition metal dichalcogenides bear great potential for photodetection and light harvesting due to high absorption coefficients. However, these applications require dissociation of strongly bound photogenerated excitons. The dissociation can be achieved by vertically stacking different monolayers to realize band alignment that favors interlayer charge transfer. In such heterostructures, the reported recombination times vary strongly, and the charge separation and recombination mechanisms remain elusive. We use two color pump–probe microscopy to demonstrate that the charge separation in a MoSe2/WSe2 heterostructure is ultrafast (∼200 fs) and virtually temperature independent, whereas the recombination accelerates strongly with temperature. Ab initio quantum dynamics simulations rationalize the experiments, indicating that the charge separation is temperature-independent because it is barrierless, involves dense acceptor states, and is promoted by higher-frequency out-of-plane vibrations. The strong temperature dependence of the recombination, on the other hand, arises from a transient indirect-to-direct bandgap modulation by low-frequency shear and layer breathing motions.