Enhanced second-harmonic generation by single metal–insulator multilayered nanocavities with axial symmetry resonating in the near-infrared

in Proceedings of SPIE: The International Society for Optical Engineering (2021), 11770

We report efficient second-harmonic emission by single multilayer metal–dielectric nanocavities. Engineering the intrinsic interface-induced symmetry breaking by resonant optical absorption design, allows ... [more ▼]

We report efficient second-harmonic emission by single multilayer metal–dielectric nanocavities. Engineering the intrinsic interface-induced symmetry breaking by resonant optical absorption design, allows to achieve almost two orders of magnitude higher second-harmonic generation efficiency compared to gold nanostructures with the same geometry. We estimate a second-order nonlinear susceptibility of the order of 1 pm/V, which is comparable to widely used nonlinear crystals. We envision that our system, which combines the advantages of both plasmonic and dielectric materials, might enable the realization of composite nano-systems for an efficient multi-purpose manipulation of nonlinear optical processes at the nanoscale. [less ▲]

Intravalley Spin-Flip Relaxation Dynamics in Single-Layer WS2

in NANO LETTERS (2018), 18(11), 6882-6891

In monolayer (1L) transition metal dichalcogenides (TMDs) the valence and conduction bands are spin-split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the ... [more ▼]

In monolayer (1L) transition metal dichalcogenides (TMDs) the valence and conduction bands are spin-split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the conduction band is such that the so-called dark excitons, consisting of electrons and holes with opposite spin orientation, have lower energy than A excitons. The transition from bright to dark excitons involves the scattering of electrons from the upper to the lower conduction band at the K point of the Brillouin zone, with detrimental effects for the optoelectronic response of 1L-TMDs, since this reduces their light emission efficiency. Here, we exploit the valley selective optical selection rules and use two-color helicity-resolved pump-probe spectroscopy to directly measure the intravalley spin-flip relaxation dynamics in 1L-WS2. This occurs on a sub-ps time scale, and it is significantly dependent on temperature, indicative of phonon-assisted relaxation. Time-dependent ab initio calculations show that intravalley spin-flip scattering occurs on significantly longer time scales only at the K point, while the occupation of states away from the minimum of the conduction band significantly reduces the scattering time. Our results shed light on the scattering processes determining the light emission efficiency in optoelectronic and photonic devices based on 1L-TMDs. [less ▲]