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Knowledge of the structure–property relationships of functional nanomaterials, including, for example, their size- and composition-dependent photoluminescence (PL) and particle-to-particle variations, is crucial for their design and reproducibility. Herein, the Angstrom-resolution capability of an analytical ultracentrifuge combined with an in-line multiwavelength emission detection system (MWE-AUC) for measuring the sedimentation coefficient-resolved spectrally corrected PL spectra of dispersed nanoparticles is demonstrated. The capabilities of this technique are shown for giant-shell CdSe/CdS quantum dots (g-QDs) with a PL quantum yield (PL QY) close to unity capped with oleic acid and oleylamine ligands. The MWE-AUC PL measurements are calibrated and validated with certified fluorescence standards. The spectrally corrected and size-dependent PL spectra of the g-QDs derived from a single MWE-AUC experiment are then analyzed and compared with the results of single-particle spectroscopic studies, yielding the PL spectra, decay kinetics, and blinking behavior of individual g-QDs. This study underlines the vast potential of MWE-AUC with in-line optical detection for the characterization of advanced nanomaterials with a complex structure.
We present colloidally stable and highly luminescent ZnxCd1_xS:Mn/ZnS core–shell nanocrystals (NCs) synthesized via a simple non-injection one-pot, two-step synthetic route, which can be easily upscaled. A systematic variation of the reaction component, parameters and thickness of the ZnS shell yielded doped nanocrystals with a very high photoluminescence quantum yield (pl) of 70%, which is the highest value yet reported for these Mn-doped sulfide-semiconductor NCs. These materials can be synthesized with high reproducibility in large quantities of the same high quality, i.e., the same pl using accordingly optimized reaction conditions. The application of these zero-reabsorption high quality NCs in the light conversion layers, deposited on top of a commercial monocrystalline silicon (mono-Si) solar cell, led to a significant enhancement of the external quantum efficiency (EQE) of this device in the ultraviolet spectral region between 300 and 400 nm up to ca. 12%. EQE enhancement is reflected by an increase in the power conversion efficiency (PCE) by nearly 0.5 percentage points and approached the theoretical limit (0.6%) expected from down-shifting for this Si solar cell. The resulting PCE may result in a BoM (bill of materials) cost reduction of app. 3% for mono-Si photovoltaic modules. Such small but distinct improvements are expected to pave the road for an industrial application of doped semiconductor NCs as cost-effective light converters for silicon photovoltaic (PV) and other optoelectronic applications.
