Surface-Mediated Tunable Self-Assembly of Single Crystal Semimetallic ErSb/GaSb Nanocomposite Structures
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Living organisms make extensive use of micro- and nanometre-sized pores as gatekeepers for controlling the movement of fluids, vapours and solids between complex environments. The ability of such pores to coordinate multiphase transport, in a highly selective and subtly triggered fashion and without clogging, has inspired interest in synthetic gated pores for applications ranging from fluid processing to 3D printing and lab-on-chip systems(1-10). But although specific gating and transport behaviours have been realized by precisely tailoring pore surface chemistries and pore geometries(6,11-17), a single system capable of controlling complex, selective multiphase transport has remained a distant prospect, and fouling is nearly inevitable(11,12). Here we introduce a gating mechanism that uses a capillary-stabilized liquid as a reversible, reconfigurable gate that fills and seals pores in the closed state, and creates a non-fouling, liquid-lined pore in the open state. Theoretical modelling and experiments demonstrate that for each transport substance, the gating threshold-the pressure needed to open the pores-can be rationally tuned over a wide pressure range. This enables us to realize in one system differential response profiles for a variety of liquids and gases, even letting liquids flow through the pore while preventing gas from escaping. These capabilities allow us to dynamically modulate gas-liquid sorting in a microfluidic flow and to separate a three-phase air-water-oil mixture, with the liquid lining ensuring sustained antifouling behaviour. Because the liquid gating strategy enables efficient long-term operation and can be applied to a variety of pore structures and membrane materials, and to micro- as well as macroscale fluid systems, we expect it to prove useful in a wide range of applications.
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The strength of electrostatic interactions within semiconductors strongly affects their performance in optoelectronic devices. An important target is the tuning of a material’s exciton binding energy—the energy binding an electron–hole pair through the electrostatic Coulomb force—independent of its electronic band gap. Here, we report on the doping of a family of two-dimensional hybrid perovskites, in which inorganic lead halide sheets alternate with naphthalene-based organic layers, with tetrachloro-1,2-benzoquinone (TCBQ). For four out of seven n = 1 perovskites, the incorporation of the electron-accepting TCBQ dopant into the organic sublattice containing the electron-donating naphthalene species enabled the tuning of the materials’ 1s exciton binding energy. The naphthalene–TCBQ electron donor–acceptor interactions increased the electrostatic screening of the exciton, in turn lowering its binding energy relative to the undoped perovskite—by almost 50% in one system. Structural and optical characterization showed that the inorganic lattice is not significantly perturbed even though the layer-to-layer spacing increases upon molecular dopant incorporation.
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Due to the prominent characteristics of carbon-based luminescent nanostructures (known colloquially as carbon dots), such as inexpensive precursors, excellent hydrophilicity, low toxicity, and intrinsic fluorescence, these nanomaterials are regarded as potential candidates to replace traditional quantum dots in some applications. As such, research in the field of carbon dots has been increasing in recent years. In this mini-review, we summarize recent progress in studies of multicolor carbon dots focusing on potential photoluminescence mechanisms, strategies for effective syntheses, and applications in ion/molecule and temperature sensing, and high-resolution bioimaging techniques.
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Thermoresponsive hydrogels have been studied intensively for creating smart drug carriers and controlled drug delivery. Understanding the drug release kinetics and corresponding transport mechanisms of nanoparticles (NPs) in a thermoresponsive hydrogel network is the key to the successful design of smart drug delivery systems. Here, we construct a mesoscopic model of rigid NPs entrapped in a hydrogel network in an aqueous solution, where the hydrogel network is formed by cross-linked semiflexible polymers of thermoresponsive poly(N-isopropylacrylamide) (PNIPAM). By varying the temperature crossing the lower critical solution temperature of PNIPAM, we can significantly change the hydrogel network characteristics. We systematically investigate how the matrix porosity and the nanoparticle size affect the transport kinetics of NPs at different temperatures. Quantitative results on the mean-squared displacement and the van Hove displacement distributions of NPs show that all NPs entrapped in the smart hydrogels undergo subdiffusion at both low and high temperatures. For a coil state, the transport of NPs in the hydrogels can be enhanced by decreasing the matrix porosity of the polymer network and NPs' size. However, when the solution temperature is increased above the critical temperature, the hydrogel network collapses following the coil-to-globule transition, with the NPs tightly trapped in some local regions inside the hydrogels. Consequently, the NP diffusion coefficient can be reduced by two orders of magnitude, or the diffusion processes can even be completely stopped. These findings provide new insights for designing controlled drug release from stimuli-responsive hydrogels, including autonomously switch on/off drug release in response to physical and chemical stimuli.
Omniphobic surfaces that can repel fluids at temperatures higher than 100 degrees C are rare. Most state-of-the-art liquid-repellent materials are based on the lotus effect, where a thin air layer is maintained throughout micro/nanotextures leading to high mobility of liquids. However, such behavior eventually fails at elevated temperatures when the surface tension of test liquids decreases significantly. Here, we demonstrate a class of lubricant-infused structured surfaces that can maintain a robust omniphobic state even for low-surface-tension liquids at temperatures up to at least 200 degrees C. We also demonstrate how liquid mobility on such surfaces can be tuned by a factor of 1000. (C) 2013 Author(s).
Pure and Sn doped ZnO nanostructures have been grown on SiO{sub 2}/Si substrates by vapor-solid technique without using any catalysts. It has been found that the morphology of the nanostructures depend strongly on the growth temperature and doping concentration. By proper tuning of the growth temperature, morphology of pure ZnO can be changed from tetrapods to multipods. On the other hand, by varying the doping concentration of Sn in ZnO, the morphology can be tuned from tetrapods to flower-like multipods to nanowires. X-ray diffraction pattern reveals that the nanostructures have a preferred (0002) growth orientation, and they are tensile strained with the increase of Sn doping in ZnO. Temperature-dependent photoluminescence characteristics of these nanostructures have been investigated in the range from 10 to 300 K. Pure ZnO tetrapods exhibited less defect state emissions than that of pure ZnO multipods. The defect emission is reduced with low concentration of Sn doping, but again increases at higher concentration of doping because of increased defects. Transport properties of pure and Sn doped ZnO tetrapods have been studied using complex-plane impedance spectroscopy. The contribution from the arms and junctions of a tetrapod could be distinguished. Sn doped ZnO samples showed lower conductivity but higher relaxation time than that of pure ZnO tetrapods.
We study the statistics of the amplitude of the synchronization error in chaotic electronic circuits coupled through linear feedback. Depending on the coupling strength, our system exhibits three qualitatively different regimes of synchronization: weak coupling yields independent oscillations; moderate to strong coupling produces a regime of intermittent synchronization known as attractor bubbling; and stronger coupling produces complete synchronization. In the regime of moderate coupling, the probability distribution for the sizes of desynchronization events follows a power law, with an exponent that can be adjusted by changing the coupling strength. Such power-law distributions are interesting, as they appear in many complex systems. However, most of the systems with such a behavior have a fixed value for the exponent of the power law, while here we present an example of a system where the exponent of the power law is easily tuned in real time.
Stable n-doping of WSe{sub 2} using thin films of SiN{sub x} deposited on the surface via plasma-enhanced chemical vapor deposition is presented. Positive fixed charge centers inside SiN{sub x} act to dope WSe{sub 2} thin flakes n-type via field-induced effect. The electron concentration in WSe{sub 2} can be well controlled up to the degenerate limit by simply adjusting the stoichiometry of the SiN{sub x} through deposition process parameters. For the high doping limit, the Schottky barrier width at the metal/WSe{sub 2} junction is significantly thinned, allowing for efficient electron injection via tunneling. Using this doping scheme, we demonstrate air-stable WSe{sub 2} n-MOSFETs with a mobility of ∼70 cm{sup 2}/V s.
The spin crossover (SCO) transitions at both the surface and over the entire volume of the [Fe{H2B(pz)(2)}(2) (bipy)] polycrystalline films on Al2O3 substrates have been studied, where pz = pyrazol-1-yl and bipy = 2,2'-bipyridine. For [Fe{H2B(pz)(2)}(2) (bipy)] films of hundreds of nm thick, magnetometry and x-ray absorption spectroscopy measurements show thermal hysteresis in the SCO transition with temperature, although the transition in bulk [Fe{H2B(pz)(2)}(2) (bipy)] occurs in a non-hysteretic fashion at 157K. While the size of the crystallites in those films are similar, the hysteresis becomes more prominent in thinner films, indicating a significant effect of the [Fe{H2B(pz)(2)}(2)(bipy)]/Al2O3 interface. Bistability of spin states, which can be inferred from the thermal hysteresis, was directly observed using temperature-dependent x-ray diffraction; the crystallites behave as spin-state domains that coexist during the transition. The difference between the spin state of molecules at the surface of the [Fe{H2B(pz)(2)}(2)(bipy)] films and that of the molecules within the films, during the thermal cycle, indicates that both cooperative (intermolecular) effects and coordination are implicated in perturbations to the SCO transition.