Colloidal nanocrystals of fully inorganic cesium lead halide (CsPbX3, X = Cl, Br, I, or combinations thereof) perovskites have attracted much attention for photonic and optoelectronic applications. Herein, we demonstrate a facile room-temperature (e.g., 25 °C), ligand-mediated reprecipitation strategy for systematically manipulating the shape of CsPbX3 colloidal nanocrystals, such as spherical quantum dots, nanocubes, nanorods, and nanoplatelets. The colloidal spherical quantum dots of CsPbX3 were synthesized with photoluminescence (PL) quantum yield values up to >80%, and the corresponding PL emission peaks covering the visible range from 380 to 693 nm. Besides spherical quantum dots, the shape of CsPbX3 nanocrystals could be engineered into nanocubes, one-dimensional nanorods, and two-dimensional few-unit-cell-thick nanoplatelets with well-defined morphology by choosing different organic acid and amine ligands via the reprecipitation process. The shape-dependent PL decay lifetimes have been determined to be several to tens to hundreds of nanoseconds. Our method provides a facile and versatile route to rationally control the shape of the CsPbX3 perovskites nanocrystals, which will create opportunities for applications such as displays, lasing, light-emitting diodes, solar concentrators, and photon detection.
We present a strategy to design and construct self-assembling DNA nanostructures that define intricate curved surfaces in three-dimensional (3D) space using the DNA origami folding technique. Double-helical DNA is bent to follow the rounded contours of the target object, and potential strand crossovers are subsequently identified. Concentric rings of DNA are used to generate in-plane curvature, constrained to 2D by rationally designed geometries and crossover networks. Out-of-plane curvature is introduced by adjusting the particular position and pattern of crossovers between adjacent DNA double helices, whose conformation often deviates from the natural, B-form twist density. A series of DNA nanostructures with high curvature--such as 2D arrangements of concentric rings and 3D spherical shells, ellipsoidal shells, and a nanoflask--were assembled.
Recently, the pursuit of high photoluminescence quantum yields (PLQYs) for blue emission in perovskite nanocrystals (NCs) has attracted increased attention because the QY of blue NCs lags behind those of green and red ones severely, which is fatal for three-primary-color displays. Here, we propose an in situ PbBr 6 4− octahedra passivation strategy to achieve a 96% absolute QY for the ultrapure (line width = 12 nm) blue emission from CsPbBr 3 nanoplatelets (NPLs), and both values rank first among perovskite NCs with blue emission. From the aspect of constructing intact PbBr 6 4− octahedra, additional Br − was introduced to drive the ionic equilibrium to form intact Pb−Br octahedra. The reduced Br vacancy and inhibited nonradiative recombination processes are well proved by reduced Urbach energy, increased Pb−Br bonds, and slower transient absorption delay. Blue light-emitting diodes (LEDs) using NPLs were fabricated, and a high external quantum efficiency (EQE) of 0.124% with an emission line width of ∼12 nm was realized. This work will provide good references to break the "blue-wall" in perovskite NCs.
Here we demonstrate Au nanoparticle self-similar chain structure organized by triangle DNA origami with well-controlled orientation and <10 nm spacing. We show for the first time that a large DNA complex (origami) and multiple AuNP conjugates can be well-assembled and purified with reliable yields. The assembled structure could be used to generate high local-field enhancement. The same method can be used to precisely localize multiple components on a DNA template for potential applications in nanophotonic, nanomagnetic, and nanoelectronic devices.
Many natural underwater adhesives harness hierarchically assembled amyloid nanostructures to achieve strong and robust interfacial adhesion under dynamic and turbulent environments. Despite recent advances, our understanding of the molecular design, self-assembly, and structure-function relationship of those natural amyloid fibers remains limited. Thus, designing biomimetic amyloid-based adhesives remains challenging. Here, we report strong and multi-functional underwater adhesives obtained from fusing mussel foot proteins (Mfps) of Mytilus galloprovincialis with CsgA proteins, the major subunit of Escherichia coli amyloid curli fibers. These hybrid molecular materials hierarchically self-assemble into higher-order structures, in which, according to molecular dynamics simulations, disordered adhesive Mfp domains are exposed on the exterior of amyloid cores formed by CsgA. Our fibers have an underwater adhesion energy approaching 20.9 mJ/m2, which is 1.5 times greater than the maximum of bio-inspired and bio-derived protein-based underwater adhesives reported thus far. Moreover, they outperform Mfps or curli fibers taken on their own at all pHs and exhibit better tolerance to auto-oxidation than Mfps at pH ≥7.0. This work establishes a platform for engineering multi-component self-assembling materials inspired by nature.
Colloidal nanocrystals of lead halide perovskites have recently received great attention due to their remarkable performance in optoelectronic applications (e.g., light-emitting devices, flexible electronics, and photodetectors). However, the use of lead remains of great concern due to its toxicity and bioaccumulation in the ecosystem; herein we report a strategy to address this issue by using tetravalent tin (Sn 4+ ) instead of divalent lead (Pb 2+ ) to synthesize stable Cs 2 SnI 6 perovskite nanocrystals. The shapes of assynthesized Cs 2 SnI 6 nanocrystals are tuned from spherical quantum dots, nanorods, nanowires, and nanobelts to nanoplatelets via a facile hot-injection process using inexpensive and nontoxic commercial precursors. Spherical aberration corrected scanning transmission electron microscopy (Cs-corrected STEM) and simulation studies revealed a well-defined face-centered-cubic (fcc) perovskite derivative structure of Cs 2 SnI 6 nanocrystals. The solution-processed Cs 2 SnI 6 nanocrystal-based field effect transistors (FETs) displayed a p-type semiconductor behavior with high hole mobility (>20 cm 2 /(V s)) and high I-ON/I-OFF ratio (>10 4 ) under ambient conditions. We envision that this work will pave the way to produce new families of high-performance, stable, low-cost and nontoxic nanocrystals for optoelectronic applications.
Many natural biological systems - such as biofilms, shells and skeletal tissues - are able to assemble multifunctional and environmentally responsive multiscale assemblies of living and non-living components. Here, by using inducible genetic circuits and cellular communication circuits to regulate Escherichia coli curli amyloid production, we show that E. coli cells can organize self-assembling amyloid fibrils across multiple length scales, producing amyloid-based materials that are either externally controllable or undergo autonomous patterning. We also interfaced curli fibrils with inorganic materials, such as gold nanoparticles (AuNPs) and quantum dots (QDs), and used these capabilities to create an environmentally responsive biofilm-based electrical switch, produce gold nanowires and nanorods, co-localize AuNPs with CdTe/CdS QDs to modulate QD fluorescence lifetimes, and nucleate the formation of fluorescent ZnS QDs. This work lays a foundation for synthesizing, patterning, and controlling functional composite materials with engineered cells.
We report the possible mechanism of forming of CdSe nanocrystals in the high boiling point solvents with long alkane chains and a novel Non-TOP-Based route to zinc-blende CdSe nanocrystals. A new mechanism shows that there exits a redox reaction in the long alkane chain solvents: Se is reduced to H2Se gas; at the same time, the long alkane chains are oxidated to alkene chains; then, the Cd complex reacts with H2Se to form CdSe nanocrystals. Possible chemical reaction equations involved in the process of forming the CdSe nanocrystals have been discussed. The alkene chain and H2Se were detected respectively by a series of experiments to support the new mechanism. Under the guidance of this mechanism, we have developed a much cheaper and greener Non-TOP-Based route for the synthesis of a size series of high-quality zinc-blende (cubic) CdSe nanocrystals. Low-cost, green, and environmentally friendlier reagents are used, without use of expensive solvents such as trioctylphosphine (TOP) or tributylphosphine (TBP). The new route enables us to achieve high-quality CdSe nanocrystals with sharp ultraviolet and visible (UV-vis) absorption peaks, controllable size (2.0-5.0 nm), bright photoluminescence (PL), narrow PL full width of half-maximum (fwhm) (29-48 nm), and high PL quantum yield (up to 60%) without any size sorting.
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