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While luminescent concentrators (LCs) are mainly designed to harvest sunlight and convert its energy into electricity, the same concept can be advantageous in alternative applications. Examples of such applications are demonstrated here by coupling the edge-guided light of high-performance LCs based on CuInSe x S 2 - x /ZnS quantum dots into optical fibers with emission covering visible-to-NIR spectral regions. In particular, a cost-efficient, miniature broadband light source for medical diagnostics, a spectral-conversion and light-guiding device for agriculture, and a large-area broadband tunable detector for telecommunications are demonstrated. Various design considerations and performance optimization approaches are discussed and summarized. Prototypes of the devices are manufactured and tested. Individual elements of the broadband light source show coupling efficiencies up to 1%, which is sufficient to saturate typical fiber-coupled spectrometers at a minimal integration time of 1 ms using 100 mW blue excitation. Agricultural devices are capable of delivering ∼10% of photosynthetically active radiation (per device) converted from absorbed sunlight to the lower canopy of plants, which boosted the tomato yield in a commercial greenhouse by 7% (fresh weight). Finally, large-scale prototype detectors can be used to discern time-modulated unfocused signals with an average power as low as 1 μW, which would be useful for free-space telecommunication systems. Fully optimized devices are expected to make significant impacts on speed and bandwidth of free-space telecommunication systems, medical diagnostics, and greenhouse crop yields.

We report size-dependent exciton formation dynamics within colloidal silicon quantum dots (Si QDs) using time-resolved terahertz (THz) spectroscopy measurements. THz photoconductivity measurements are used to distinguish the initially created hot carriers from excitons that form at later times. At early pump/probe delays, the exciton formation dynamics are revealed by the temporal evolution of the THz transmission. We find an increase in the exciton formation time, from ∼500 to ∼900 fs, as the Si QD diameter is reduced from 7.3 to 3.4 nm and all sizes exhibit slower hot-carrier relaxation times compared to bulk Si. In addition, we determine the THz absorption cross section at early delay times is proportional to the carrier mobility while at later delays is proportional to the exciton polarizability, αX. We extract a size-dependent αX and find an ∼r(4) dependence, consistent with previous reports for quantum-confined excitons in CdSe, InAs, and PbSe QDs. The observed slowing in exciton formation time for smaller Si QDs is attributed to decreased electron-phonon coupling due to increased quantum confinement. These results experimentally verify the modification of hot-carrier relaxation rates by quantum confinement in Si QDs, which likely plays a significant role in the high carrier multiplication efficiency observed in these nanomaterials.

We simultaneously determined the charge carrier mobility and picosecond to nanosecond carrier dynamics of isolated silicon nanowires (Si NWs) and nanocrystals (Si NCs) using time-resolved terahertz spectroscopy. We then compared these results to data measured on bulk c-Si as a function of excitation fluence. We find >1 ns carrier lifetimes in Si NWs that are dominated by surface recombination with surface recombination velocities (SRV) between ∼1100-1700 cm s(-1) depending on process conditions. The Si NCs have markedly different decay dynamics. Initially, free-carriers are produced, but relax within ∼1.5 ps to form bound excitons. Subsequently, the excitons decay with lifetimes >7 ns, similar to free carriers produced in bulk Si. The isolated Si NWs exhibit bulk-like mobilities that decrease with increasing excitation density, while the hot-carrier mobilities in the Si NCs are lower than bulk mobilities and could only be measured within the initial 1.5 ps decay. We discuss the implications of our measurements on the utilization of Si NWs and NCs in macroscopic optoelectronic applications.

We have synthesized alkylselenide reagents to replace the native oleate ligand on PbSe quantum dots (QDs) in order to investigate the effect of surface modification on their stoichiometry, photophysics, and air stability. The alkylselenide reagent removes all of the oleate on the QD surface and results in Se addition; however, complete Se enrichment does not occur, achieving a 53% decrease in the amount of excess Pb for 2 nm diameter QDs and a 23% decrease for 10 nm QDs. Our analysis suggests that the Se ligand preferentially binds to the {111} faces, which are more prevalent in smaller QDs. We find that attachment of the alkylselenide ligand to the QD surface enhances oxidative resistance, likely resulting from a more stable bond between surface Pb atoms and the alkylselenide ligand compared to Pb-oleate. However, binding of the alkylselenide ligand produces a separate nonradiative relaxation route that partially quenches PL, suggesting the formation of a dark hole-trap.