Temporal color mixing and dynamic beam shaping with silicon metasurfaces.

Metasurfaces offer the possibility to shape optical wavefronts with an ultracompact, planar form factor. However, most metasurfaces are static, and their optical functions are fixed after the fabrication process. Many modern optical systems require dynamic manipulation of light, and this is now driving the development of electrically reconfigurable metasurfaces. We can realize metasurfaces with fast (>105 hertz), electrically tunable pixels that offer complete (0- to 2π) phase control and large amplitude modulation of scattered waves through the microelectromechanical movement of silicon antenna arrays created in standard silicon-on-insulator technology. Our approach can be used to realize a platform technology that enables low-voltage operation of pixels for temporal color mixing and continuous, dynamic beam steering and light focusing.

Type-tunable amplified spontaneous emission from core-seeded CdSe/CdS nanorods controlled by exciton-exciton interaction.

Type-tunable optical gain performance of core-seeded CdSe/CdS nanorods is studied via two-photon optical pumping. Controlling the exciton-exciton interaction by varying the core and shell size, blue-shifted and red-shifted modes of amplified spontaneous emission are systematically demonstrated and their type attributions are verified by time-resolved emission kinetics.

Nanocrystal skins with exciton funneling for photosensing.

Highly photosensitive nanocrystal (NC) skins based on exciton funneling are proposed and demonstrated using a graded bandgap profile across which no external bias is applied in operation for light-sensing. Four types of gradient NC skin devices (GNS) made of NC monolayers of distinct sizes with photovoltage readout are fabricated and comparatively studied. In all structures, polyelectrolyte polymers separating CdTe NC monolayers set the interparticle distances between the monolayers of ligand-free NCs to <1 nm. In this photosensitive GNS platform, excitons funnel along the gradually decreasing bandgap gradient of cascaded NC monolayers, and are finally captured by the NC monolayer with the smallest bandgap interfacing the metal electrode. Time-resolved measurements of the cascaded NC skins are conducted at the donor and acceptor wavelengths, and the exciton transfer process is confirmed in these active structures. These findings are expected to enable large-area GNS-based photosensing with highly efficient full-spectrum conversion.

Observation of biexcitons in nanocrystal solids in the presence of photocharging.

In nanocrystal quantum dots (NQDs), generating multiexcitons offers an enabling tool for enhancing NQD-based devices. However, the photocharging effect makes understanding multiexciton kinetics in NQD solids fundamentally challenging, which is critically important for solid-state devices. To date, this lack of understanding and the spectral-temporal aspects of the multiexciton recombination still remain unresolved in solid NQD ensembles, which is mainly due to the confusion with recombination of carriers in charged NQDs. In this work, we reveal the spectral-temporal behavior of biexcitons (BXs) in the presence of photocharging using near-unity quantum yield CdSe/CdS NQDs exhibiting substantial suppression of Auger recombination. Here, recombinations of biexcitons and single excitons (Xs) are successfully resolved in the presence of trions in the ensemble measurements of time-correlated single-photon counting at variable excitation intensities and varying emission wavelengths. The spectral behaviors of BXs and Xs are obtained for three NQD samples with different core sizes, revealing the strength tunability of the X-X interaction energy in these NQDs. The extraction of spectrally resolved X, BX, and trion kinetics, which are otherwise spectrally unresolved, is enabled by our approach introducing integrated time-resolved fluorescence. The results are further experimentally verified by cross-checking excitation intensity and exposure time dependencies as well as the temporal evolutions of the photoluminescence spectra, all of which prove to be consistent. The BX and X energies are also confirmed by theoretical calculations. These findings fill an important gap in understanding the spectral dynamics of multiexcitons in such NQD solids under the influence of photocharging effects, paving the way to engineering of multiexciton kinetics in nanocrystal optoelectronics, including NQD-based lasing, photovoltaics, and photodetection.