Two-dimensional (2D) sheets are currently in the spotlight of nanotechnology owing to high-performance device fabrication possibilities. Building a free-standing quantum sheet with controlled morphology is challenging when large planar geometry and ultranarrow thickness are simultaneously concerned. Coalescence of nanowires into large single-crystalline sheet is a promising approach leading to large, molecularly thick 2D sheets with controlled planar morphology. Here we report on a bottom-up approach to fabricate high-quality ultrathin 2D single crystalline sheets with well-defined rectangular morphology via collective coalescence of PbS nanowires. The ultrathin sheets are strictly rectangular with 1.8 nm thickness, 200-250 nm width, and 3-20 μm length. The sheets show high electrical conductivity at room and cryogenic temperatures upon device fabrication. Density functional theory (DFT) calculations reveal that a single row of delocalized orbitals of a nanowire is gradually converted into several parallel conduction channels upon sheet formation, which enable superior in-plane carrier conduction.
In-plane compressively strained α-Sn films have been theoretically predicted and experimentally proven to possess nontrivial electronic states of a 3D topological Dirac semimetal. The robustness of these states typically strongly depends on purity, homogeneity and stability of the grown material itself. By developing a reliable fabrication process, we were able to grow pure strained α-Sn films on InSb(100), without heating of the substrate during growth, nor using any dopants. The α-Sn films were grown by molecular beam epitaxy, followed by experimental verification of the achieved chemical purity and structural properties of the film's surface. Local insight into the surface morphology was provided by scanning tunneling microscopy. We detected the existence of compressive strain using Mössbauer spectroscopy and we observed a remarkable robustness of the grown samples against ambient conditions. The topological character of the samples was confirmed by angle-resolved photoemission spectroscopy, revealing the Dirac cone of the topological surface state. Scanning tunneling spectroscopy, moreover, allowed obtaining an improved insight into the electronic structure of the 3D topological Dirac semimetal α-Sn above the Fermi level.
Graphene quantum dots (GQDs) have attracted a large amount of attention due to their unique optoelectronic properties, which arise from the quantum confinement effect or edge effect or surface functionalization. Popular routes for designing GQDs are based on the reactions in aqueous phases, which are detrimental for integration of GQDs into optoelectronic devices. Hence, a critical challenge remains in utilizing the water-soluble GQDs for fabricating optoelectronic devices. Here we demonstrate for the first time a single step facile route to extract water-soluble GQDs into solid powder under reduced pressure for the fabrication of light emitting diodes (LEDs). The process avoids the need for post synthesis ex situ functionalization or the use of additional polymers to make GQDs hydrophobic retaining the intrinsic luminescent behavior of GQDs. The measured current-voltage characteristics of GQD-LED devices showed a significantly low turn-on voltage of $2.5 V. Bias dependent electroluminescence leading to color tunability from blue to deep cyan is demonstrated.
Monocomponent quantum dots (QDs) possess limited electron−hole delocalization capacity upon photoexcitation that suppresses the efficiency of photoenergy harvesting devices. Type II heterostructures offer band offsets at conduction and valence bands depending upon the band gaps of the constituent QDs which largely depend on their sizes. Hence, by keeping the size of one constituent QD fixed while varying the size of the other QD selectively, the band offsets at the interface can be engineered selectively. We report on the tuning of band offsets by synthesizing component size modulated heterostructures composed of a fixed sized ZnSe QD and size tuned CdS QDs with variable band gaps. The resultant heterostructures show spontaneous charge carrier separation across the interface upon photoexcitation depending on the extent of band offsets. Formation mechanism, epitaxial relationship, and the intrinsic nature of interface of the heterostructures are investigated. Experimental results are corroborated with ab initio electronic structure calculations based on density functional theory. Spontaneous charge carrier delocalization across the interface depends on the magnitude of band offsets, which facilitates fabrication of QD sensitized solar cells (QDSSCs). Improved device performances of QDSSCs in comparison to the limited photon-to-current conversion efficiencies of monocomponent QDs demonstrates the significance of band offsets for natural charge carrier separation.
Artificial enzyme mimetics have attracted immense interest recently because natural enzymes undergo easy denaturation under environmental conditions restricting practical usefulness. We report for the first time chalcopyrite CuZnFeS (CZIS) alloyed nanocrystals (NCs) as novel biomimetic catalysts with efficient intrinsic peroxidase-like activity. Novel peroxidase activities of CZIS NCs have been evaluated by catalytic oxidation of the peroxidase substrate 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H2O2). CZIS NCs demonstrate the synergistic effect of elemental composition and photoactivity towards peroxidase-like activity. The quaternary CZIS NCs show enhanced intrinsic peroxidase-like activity compared to the binary NCs with the same constituent elements. Intrinsic peroxidase-like activity has been correlated with the energy band position of CZIS NCs extracted using scanning tunneling spectroscopy and ultraviolet photoelectron spectroscopy. Kinetic analyses indicate Michaelis-Menten enzyme kinetic model catalytic behavior describing the rate of the enzymatic reaction by correlating the reaction rate with substrate concentration. Typical color reactions arising from the catalytic oxidation of TMB over CZIS NCs with H2O2 have been utilized to establish a simple and sensitive colorimetric assay for detection of H2O2 and glucose. CZIS NCs are recyclable catalysts showing high efficiency in multiple uses. Our study may open up the possibility of designing new photoactive multi-component alloyed NCs as enzyme mimetics in biotechnology applications.
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