Reduced dimensionality of structures such as 0D quantum dots, 1D nanorods, and 2D nanoplatelets is predicted to favor the creation of tightly bound excitons stable at room temperature, making experimental determination of the exciton binding energy (R x ) crucial for evaluating the performance of semiconductor nanoparticles. We propose a fully optical approach for R x determination based on a complementary combination of photoacoustic and transmission spectra, using 5.5, 4.5, and 3.5 ML CdSe nanoplatelets as a benchmark system. The absence of excitonic features in photoacoustic spectra allows for probing the band-to-band transition, leading to the band gap determination. Such an unusual effect is explained by efficient re-emission of the absorbed radiation typical for high quantum yield structures, keeping the crystal lattice from excess phonon generation. The determined exciton binding energy for CdSe nanoplatelets ranges from 130 to 230 meV, confirming the presence of robust excitons in highly confined 2D systems.
Nonlinear optical processes are crucial for emerging applications including multiphoton-excited fluorescence microscopy and optical power limiting. Therefore, searching for materials of high multiphoton absorption cross sections is essential for the development of these techniques. We present synthesis of 4.5 monolayer CdSe nanoplatelets (NPLs) doped with silver and copper ions along with the evaluation of their two-photon absorption (TPA) and three-photon absorption (3PA) cross sections. Doping significantly increases the TPA cross section of each NPL sample, which reaches up to 1.33 × 10 7 GM for the most absorbing copper-doped ones. We also detected 1−2 orders of magnitude-enhanced 3PA cross sections for the doped NPLs in comparison with their undoped counterparts. As TPA and 3PA peaks appear, in the first and the second biological transmission windows, respectively, doped NPLs are promising candidates for multiphoton fluorescence microscopy as bioimaging agents. Moreover, the strong nonlinear response suggests application as active optoelectronic materials in optical sensors.
The tuning of the spectroscopic signatures of boron-carrying fluorescent dyes by subtle chemical modifications is achieved. In more details, we propose a new series of compounds incorporating up to three...
We demonstrate a low-temperature synthesis of hydrophilic, penicillamine-stabilized hybrid CdS-Au nanoparticles (NPs) utilizing different Au concentrations. The obtained hybrid nanomaterials exhibit photoluminescence quenching and emission lifetime reduction in comparison with their raw semiconductor CdS NPs counterparts. An increase of concentration of Au present at the surface of CdS leads to lower photoluminescence intensity and faster emission decays, suggesting more efficient charge separation when larger Au domains are present. For photocatalysis studies, we performed methylene blue (MB) absorption measurements under irradiation in the presence of CdS-Au NPs. After 1 h of light exposure, we observed the absorbance decrease to about 35% and 10% of the initial value for the CdS-5Au and CdS-7.5Au (the hybrid NPs obtained in a presence of 5.0 and 7.5 mM Au), respectively, which indicates MB reduction caused by electrons effectively separated from holes on metal surface. In further similar photocatalysis experiments, we measured bovine serum albumin (BSA) integrated photoluminescence intensity quenching in the presence of CdS-Au NPs, with a 50% decrease being obtained for CdS-2.5Au NPs and CdS-5Au NPs, with a faster response rate detected for the system prepared with a higher Au concentration. The results suggest hole-driven reactive oxygen species (ROS) production, causing BSA degeneration. Finally, we performed two-photon excited emission (TPEE) measurements for CdS-5Au NPs, obtaining their two-photon absorption (TPA) cross-section values up to 15.8 × 103 GM (Goeppert-Mayer units). We conclude that the obtained water-soluble CdS-Au NPs exhibit potential triple functionalities as photocatalysts for reduction and oxidation reactions as well as materials for two-photon absorption applications, so that they may be considered as future theranostics.
Introduction Semiconductor nanoplatelets (NPLs) are promising materials for nonlinear optical microscopy since they feature good two-photon absorption (TPA) properties, narrow photoluminescence spectra and high quantum yields of luminescence. Nevertheless, the use of semiconductor NPLs is inevitably connected with concerns about heavy metal ion toxicity and their intrinsically hydrophobic character. Methods Our contribution focuses on the design and engineering of coloidal bionanomaterial consisting of two-dimensional highly luminescent CdSe semiconductor NPLs loaded into spherical and homogeneous polymeric nanocarriers (NCs) based on poly(ethylene oxide) and poly(propylene oxide) block co-polymer. The biocompatibility and usefulness of the NPLs-loaded polymeric NCs in two-photon induced bioimaging was demonstrated in vitro by cytotoxicity and two-photon microscopic studies using eukaryotic (normal fibroblasts and cancer ovarian) cells. Results The encapsulated NPLs maintain their intensive and spectrally narrow photoluminescence, as well as preserve good TPA properties, while the surrounding polymer shell imparts hydrophilic character and non-toxicity towards eukaryotic cells. Specifically, TPA cross-sections of the colloidal NCs loaded with NPLs show large values reaching up to 2.0 × 10 8 GM, with simultaneously two-photon brightness reaching 2.2 × 10 7 GM at 870 nm. MTT proliferation assay performed on cell lines treated with encapsulated NPLs revealed at least 70% viability of normal human gingival fibroblast (HGF) and cancer ovarian (MDAH-2774) cells, while the results of multiphoton imaging of murine (L-929) fibroblasts suggest that the encapsulated NPLs are capable of labelling the target cells enabling their visualization. Conclusion As a result, we obtained water dispersible and temporally stable hydrophilic NPLs-loaded NCs that offer excellent, both one- and two-photon excited fluorescence preserving optical properties of the raw hydrophobic and colloidal NPLs. The biological responses upon eukaryotic cells indicate that the encapsulation process protects cells from the toxic influence of cadmium simultaneously preserving the unique multiphoton properties of the active cargo which opens a promising perspective for its application in multiphoton cancer bioimaging excited at the “optical transmission window” of biological tissues in near-infrared range.
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