Active control of mid-wavelength infrared non-linearity in silicon photonic crystal slab.

Natural materials' inherently weak nonlinear response demands the design of artificial substitutes to avoid optically large samples and complex phase-matching techniques. Silicon photonic crystals are promising artificial materials for this quest. Their nonlinear properties can be modulated optically, paving the way for applications ranging from ultrafast information processing to quantum technologies. A two-dimensional 15-µm-thick silicon photonic structure, comprising a hexagonal array of air holes traversing the slab's thickness, has been designed to support a guided resonance for the light with a wavelength of 4-µm. At the resonance conditions, a transverse mode of the light is strongly confined between the holes in the "veins" of the silicon component. Owing to the confinement, the structure exhibits a ratio of nonlinear to linear absorption coefficients threefold higher than the uniform silicon slab of the same thickness. A customised time-resolved Z-scan method with provisions to accommodate ultrafast pump-probe measurements was used to investigate and quantify the non-linear response. We show that optically pumping free charge carriers into the structure decouples the incoming light from the resonance and reduces the non-linear response. The time-resolved measurements suggest that the decoupling is a relatively long-lived effect on the scale comparable to the non-radiative recombination in the bulk material. Moreover, we demonstrate that the excited free carriers are not the source of the nonlinearity, as this property is determined by the structure design.

Taming non-radiative recombination in Si nanocrystals interlinked in a porous network.

A range of the distinctive physical properties, comprising high surface-to-volume ratio, possibility to achieve mechanical and chemical stability after a tailored treatment, controlled quantum confinement and the room-temperature photoluminescence, combined with mass production capabilities offer porous silicon unmatched capabilities required for the development of electro-optical devices. Yet, the mechanism of the charge carrier dynamics remains poorly controlled and understood. In particular, non-radiative recombination, often the main process of the excited carrier's decay, has not been adequately comprehended to this day. Here we show, that the recombination mechanism critically depends on the composition of surface passivation. That is, hydrogen passivated material exhibits Shockley-Read-Hall type of decay, while for oxidised surfaces, it proceeds by two orders of magnitude faster and exclusively through the Auger process. Moreover, it is possible to control the source of recombination in the same sample by applying a cyclic sequence of hydrogenation-oxidation-hydrogenation processes, and, consequently switching on-demand between Shockley-Read-Hall and Auger recombinations. Remarkably, irregardless of the recombination mechanism, the rate constant scales inversely with the average volume of individual silicon nanocrystals contained in the material. Thus, the type of the non-radiative recombination is established by the composition of the passivation, while its rate depends on the degree of the charge carriers' quantum confinement.

Gold nanoplasmonic particles in tunable porous silicon 3D scaffolds for ultra-low concentration detection by SERS.

A composite material of plasmonic nanoparticles embedded in a scaffold of nano-porous silicon offers unmatched capabilities for use as a SERS substrate. The marriage of these components presents an exclusive combination of tightly focused amplification of Localised Surface Plasmon (LSP) fields inside the material with an extremely high surface-to-volume ratio. This provides favourable conditions for a single molecule or extremely low concentration detection by SERS. In this work the advantage of the composite is demonstrated by SERS detection of Methylene Blue at a concentration as low as a few picomolars. We systematically investigate the plasmonic properties of the material by imaging its morphology, establishing its composition and the effect on the LSP resonance optical spectra.

Reconstructing charge-carrier dynamics in porous silicon membranes from time-resolved interferometric measurements.

We performed interferometric time-resolved simultaneous reflectance and transmittance measurements to investigate the carrier dynamics in pump-probe experiments on thin porous silicon membranes. The experimental data was analysed by using a method built on the Wentzel-Kramers-Brillouin approximation and the Drude model, allowing us to reconstruct the excited carriers' non-uniform distribution in space and its evolution in time. The analysis revealed that the carrier dynamics in porous silicon, with ~50% porosity and native oxide chemistry, is governed by the Shockley-Read-Hall recombination process with a characteristic time constant of 375 picoseconds, whereas diffusion makes an insignificant contribution as it is suppressed by the high rate of scattering.

Determination of excitation profile and dielectric function spatial nonuniformity in porous silicon by using WKB approach.

We develop an analytical model based on the WKB approach to evaluate the experimental results of the femtosecond pump-probe measurements of the transmittance and reflectance obtained on thin membranes of porous silicon. The model allows us to retrieve a pump-induced nonuniform complex dielectric function change along the membrane depth. We show that the model fitting to the experimental data requires a minimal number of fitting parameters while still complying with the restriction imposed by the Kramers-Kronig relation. The developed model has a broad range of applications for experimental data analysis and practical implementation in the design of devices involving a spatially nonuniform dielectric function, such as in biosensing, wave-guiding, solar energy harvesting, photonics and electro-optical devices.