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            Abstract The discovery of carbon dots opens a new avenue to the applications of nanomaterials in biosensing and bioimaging. In this work, we develop simple methods to prepare carbon nanoparticles from xylose and to tune the photoluminescence (PL) characteristics of the xylose-derived carbon nanoparticles via the combination of three different processes: hydrothermal carbonization (HTC), annealing at 850 °C and laser ablation (LA) in a NH4OH solution. The HTC-synthesized carbon dots (CDs) exhibit green emission under the 365 nm UV excitation, the annealing of the HTC-synthesized CDs leads to complete loss of the PL characteristics, and the LA processing of the annealed carbon nanoparticles recovers the PL characteristics with blue shift in comparison to the HTC-synthesized CDs under the same UV excitation. the PL characteristics of the HTC-CDs and the LA-CDs are dependent on theπ-π* transition of C-containing surface-functional groups andπ-π* and n-π* transitions of N-containing surface-functional groups, respectively, which are responsible for the difference in the PL characteristics between the HTC-synthesized CDs and the LA-processed CDs. The approaches demonstrated in this work provide a viable method to introduce and tune surface-functional groups on the surface of carbon nanoparticles.more » « less
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            Abstract The development of in situ growth methods for the fabrication of high‐quality perovskite single‐crystal thin films (SCTFs) directly on hole‐transport layers (HTLs) to boost the performance of optoelectronic devices is critically important. However, the fabrication of large‐area high‐quality SCTFs with thin thickness still remains a significant challenge due to the elusive growth mechanism of this process. In this work, the influence of three key factors on in situ growth of high‐quality large‐size MAPbBr3SCTFs on HTLs is investigated. An optimal “sweet spot” is determined: low interface energy between the precursor solution and substrate, a slow heating rate, and a moderate precursor solution concentration. As a result, the as‐obtained perovskite SCTFs with a thickness of 540 nm achieve a record area to thickness ratio of 1.94 × 104 mm, a record X‐ray diffraction peak full width at half maximum of 0.017°, and an ultralong carrier lifetime of 1552 ns. These characteristics enable the as‐obtained perovskite SCTFs to exhibit a record carrier mobility of 141 cm2V−1s−1and good long‐term structural stability over 360 days.more » « less
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            Large-scale and controllable fabrication is an indispensable step for the industrialization and commercialization of halide perovskite nanocrystals, which are new-generation semiconductor materials for optoelectronic applications. Microfluidics, which provides continuous and precise synthesis, has been considered as a promising technique to fulfill this aspect. The research studies over the past decades have witnessed the advancement of microfluidics as a powerful tool in the fabrication of halide perovskite nanocrystals. In this Perspective, the state-of-the-art research based on microfluidics is introduced initially, including the synthesis of functional structures and materials, devices, as well as the interdisciplinary interactions between microfluidics and artificial intelligence and machine learning, etc. We then detail the issues and challenges in hindering progress in the above areas. Finally, we provide future directions and trends for the technology to achieve its full potential. This Perspective is expected to benefit the collective efforts between the field of nanomaterials and microfluidics in advanced manufacturing.more » « less
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            Blue emitting Sn-based lead-free halide perovskite nanocrystals (NCs) are considered to be a promising material in lighting and displays. However, industrialised fabrication of blue-emitting NCs still remains a significant challenge due to the use of toxic solvents and optical instability, not mentioning in large-scale synthesis. In this work, a green-route synthesis of blue-emitting lead-free halide perovskite Cs 2 SnCl 6 powders is developed, in which deionized water with a small amount of inorganic acid is used as the solvent and the synthesis of the Cs 2 SnCl 6 powders is achieved on a microfluidic platform. Using the Cs 2 SnCl 6 powders, we prepare Cs 2 SnCl 6 NCs via an ultrasonication process. Changing the volume ratio of the ligands (oleic acid to oleylamine) can alter the photoluminescence (PL) characteristics of the prepared NCs, including the PL-peak wavelength, PL-peak intensity and quantum yield. The highest photoluminescence quantum yield (PLQY) of 13.4% is achieved by the Cs 2 SnCl 6 NCs prepared with the volume ratio of oleic acid to oleylamine of 40 μL to 10 μL. A long-term PL stability test demonstrates that the as-synthesized Cs 2 SnCl 6 NCs can retain a stable PLQY over a period of 60 days. This work opens up a new path for a large-scale green-route synthesis of blue-emitting Sn-based lead-free NCs, such as Cs 2 SnX 6 (Cl, Br and I), towards their applications in optoelectronics.more » « less
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            Kinetic analysis of the growth behavior of perovskite CsPbBr 3 nanocrystals in a microfluidic systemUnderstanding the growth behavior of nanoparticles and semiconductor nanocrystals under dynamic environments is of profound importance in controlling the sizes and uniformity of the prepared nanoparticles and semiconductor nanocrystals. In this work, we develop a relation between the bandgap (the photoluminescence peak wavelength) of semiconductor nanocrystals and the total flow rate for the synthesis of semiconductor nanocrystals in microfluidic systems under the framework of the quantum confinement effect without the contribution of Coulomb interaction. Using this relation, we analyze the growth behavior of CsPbBr 3 nanocrystals synthesized in a microfluidic system by an antisolvent method in the temperature range of 303 to 363 K. The results demonstrate that the square of the average size of the CsPbBr 3 nanocrystals is inversely proportional to the total flow rate and support the developed relation. The activation energy for the rate process controlling the growth of the CsPbBr 3 nanocrystals in the microfluidic system is 2.05 kJ mol −1 . Increasing the synthesis temperature widens the size distribution of the CsPbBr 3 NCs prepared in the microfluidic system. The method developed in this work provides a simple approach to use photoluminescent characteristics to in situ monitor and analyze the growth of semiconductor nanocrystals under dynamic environments.more » « less
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            Carbon dots (C-dots) are a promising class of carbonaceous nanomaterials for bioimaging, catalysis, and optoelectronics. However, their applications are disrupted by recent reports that bright molecular fluorophores are co-produced in the synthesis of C-dots, in particular ones prepared through a bottom-up approach (carbon nanodots (CNDs)), commonly derived from citric acid precursors. The presence of highly emissive molecular fluorophore species obscures the true performance of CNDs and severely challenges the development of CNDs. Here we observe that the issue of molecular fluorophore impurity is still problematic for CNDs which are derived from a different type of precursor, polycylic aromatic hydrocarbons (PAHs). In this study, low-oxygen-content CNDs and small molecular fluorophores are co-produced through hydrothermal condensation of nitropyrene. Extensive and systematic characterization following column chromatographic separation and solvent-induced extraction reveals that molecular fluorophores and CNDs are clearly dissimilar in structure and optical properties. This work highlights that rigorous separation and purification steps need to be taken not only for hydrophilic CNDs but also for low-oxygen-content CNDs.more » « less
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            The applications of semiconductor nanocrystals in optoelectronics are based on the unique characteristic of quantum confinement. There is great interest to tailor the performance of optoelectronic nanodevices and systems through the control of the sizes of nanocrystals. In this work, we develop a general mathematical formulation for the growth of a crystal/particle in a liquid solution, which takes account of the combinational effect of diffusion-limited growth and reaction-limited growth, and formulate the growth equations for the size of a cubic crystal grown under three different scenarios – isothermal and isochoric conditions, isothermal growth with the evaporation and/or extraction of the solvent and isochoric growth with continuous change in temperature. For the growth of a cubic crystal under isothermal and isochoric conditions, there are three growth stages – linear growth, nonlinear growth and plateau, and the growth rate in the stage of linear growth and the final size of the cubic crystal are dependent on the degree of supersaturation. For the growth of multi-crystals with a Gaussian distribution of crystal sizes, the change of the monomer concentration in a liquid solution is dependent on the change rates of average size and the standard deviation of the crystal sizes.more » « less
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            Abstract In this work, we develop an environmental-friendly approach to produce organic-inorganic hybrid MAPbBr 3 (MA = CH 3 NH 3 ) perovskite nanocrystals (PeNCs) and PMMA-MAPbBr 3 NC films with excellent compression-resistant PL characteristics. Deionized water is used as the solvent to synthesize MAPbBr 3 powder instead of conventionally-used hazardous organic solvents. The MAPbBr 3 PeNCs derived from the MAPbBr 3 powder exhibit a high photoluminescence quantum yield (PLQY) of 93.86%. Poly(methyl methacrylate) (PMMA)-MAPbBr 3 NC films made from the MAPbBr 3 PeNCs retain ∼97% and ∼91% of initial PL intensity after 720 h aging in ambient environment at 50 °C and 70 °C, respectively. The PMMA-MAPbBr 3 NC films also exhibit compression-resistant photoluminescent characteristics in contrast to the PMMA-CsPbBr 3 NC films under a compressive stress of 1.6 MPa. The PMMA-MAPbBr 3 NC film integrated with a red emissive film and a blue light emitting source achieves an LCD backlight of ∼114% color gamut of National Television System Committee (NTSC) 1953 standard.more » « less
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