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Direct Hot-Injection Synthesis of Lead Halide Perovskite Nanocubes in Acrylic Monomers for Ultrastable and Bright Nanocrystal–Polymer Composite Films
摘要： In recent years, lead halide perovskite nanocrystals (NCs) have attracted significant attention in both fundamental research and commercial applications due to their excellent optical and optoelectrical properties. However, the protective ligands on the surface of the perovskites NCs could be easily removed after the tedious process of centrifugation, separation, and dispersion, which greatly hampers their stability against light, heat, moisture, and oxygen and limits their practical applications. Here we report a new post-processing-free strategy (i.e., without centrifugation, separation, and dispersion process) of using an UV-polymerizable acrylic monomer of lauryl methacrylate (LMA) as the solvent to synthesize CsPbBr3 NCs, and then adding polyester polyurethane acrylates oligomer, monomer (IBOA) and initiator for directly UV polymerization to fabricate NC-polymer composite films. These films exhibited an improved photoluminescence quantum yield (85-90%) than classic NC-film (40-50%), which were processed using octadecene (ODE) as the solvent for NC synthesis and post-processed for UV polymerization. Significantly, the as-fabricated films by post-processing-free strategy exhibited excellent photostability against strong Xe lamp illumination; while the other films using classic methods were quickly photo-degraded. Meanwhile, these NC-polymer composite films showed good stability against moisture and heating when aging in water at 50oC for over 200 hours. These films, along with K2SiF6:Mn4+ (KSF) phosphor emitters, were used as downconverters for blue LEDs in liquid crystal displays with a wide color gamut of 115% in the International Commission on Illumination (CIE) 1931 color space. This work provides a facile and effective strategy for the preparation of ultrastable and bright color-conversion NC films for the development of the next-generation wide color gamut displays.
关键词： display backlight,lead halide perovskite,colloidal nanocrystals,color-conversion optical films,photostability
更新于2025-11-14 17:03:37
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Stepwise Two-Photon-Induced Electron Transfer from Higher Excited States of Noncovalently Bound Porphyrin-CdS/ZnS Core/Shell Nanocrystals
摘要： There has been an increasing amount of interest in stepwise two-photon absorption (2PA)-induced photochemical reactions because of their extremely lower power thresholds compared to that of the simultaneous process and drastic reaction enhancements in some cases. However, stepwise 2PA-induced photochemical reactions were reported only in single chromophores and covalently bound bi-chromophores and there are few reports on these reactions in noncovalently bound systems because of weak electronic interactions among chromophores. This study demonstrated the stepwise 2PA-induced electron transfer from higher excited states in noncovalently bound protoporphyrin IX·CdS/ZnS core/shell nanocrystals (NCs). The electron transfer from higher excited states of porphyrin to CdS NCs successfully overcomes the activation barrier associated with the wide bandgap ZnS shell, indicating that a high reduction potential can be obtained with the stepwise 2PA process. The concept presented in this study can be applied to various noncovalently bound multi-chromophore systems to explore nonlinear photoresponses.
关键词： Nonlinear,Anti-Kasha type,colloidal nanocrystals,hybrid nanomaterial,hot electron transfer
更新于2025-09-23 15:21:01
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Probing of Thermal Transport in 50-nm Thick PbTe Nanocrystal Film by Time-Domain Thermoreflectance
摘要： Bottom-up fabrication of thermoelectric (TE) materials from colloidal nanocrystal (NC) building blocks can substantially increase their TE efficiency, e.g., by reducing lattice thermal conductivity. In this work, 10-nm spherical phase-pure oleate-capped PbTe NCs with narrow size distribution were synthesized and employed to fabricate 50-nm thick films on insulating SiO2/Si substrates. The spin-coating, with subsequent ligand exchange procedure, was applied to enhance coupling interactions between the NCs. Using dark conductivity measurements, we confirmed the semiconducting behavior and the Schottky-type electrical field-dependent conductivity mechanism in the resultant thin films. The thermal transport in the thin-film was probed by means of a time-domain thermoreflectance (TDTR) method. For this purpose, we used a customized state-of-the-art system based on a picosecond thermoreflectance instrument, which enables area-selective analysis with spatial resolution down to 5 μm. The results show that as-fabricated PbTe NC films exhibit ultralow thermal conductivity of 0.9 W m–1 K–1 at 300 K. The transport property findings suggest potential in the proposed quick and cost-effective spin-coating strategy for bottom-up fabrication of nanostructured TE films from high-quality colloidal NC building blocks.
关键词： colloidal nanocrystals,spin-coating,thermoelectric materials,thermal conductivity,time-domain thermoreflectance,PbTe
更新于2025-09-23 15:21:01
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Composition and size controlled I-V-VI semiconductor nanocrystals
摘要： Non-isovalent ternary and quaternary semiconductors (i.e., having two or more cations with different valence) have unique structural and electronic properties that are leveraged in photovoltaic, thermoelectric, and phase-change memory devices. Making these complex semiconductors in the form of colloidal nanocrystals imparts size-dependent properties and solution processability. Here, we present results on I‐V‐VI group colloidal nanocrystals. We focus on achieving sub-10 nm sizes for a wide range of I-V-VI selenide nanocrystals, including AgSbSe2, AgSb2Se3, CuSbSe2, Cu3SbSe4, AgBiSe2, and CuBiSe2. To highlight one possible application for these I-V-VI colloidal nanomaterials, we analyze the optical absorption and show that through composition and size control, this class of materials offers bandgaps in the mid- to near-IR. Absorption coefficients of AgSbSe2, CuSbSe2, and Cu3SbSe4 nanocrystals are on par with or higher than the well-studied PbS nanocrystals highlighting their potential for devices such as solar cells, (mid-)infrared photodetectors, and near-infrared bio-imaging systems.
关键词： solar cells,optical absorption,bio-imaging systems,colloidal nanocrystals,infrared photodetectors,mid- to near-IR,I-V-VI semiconductor nanocrystals,bandgaps
更新于2025-09-23 15:19:57