This study reports on "phase" transitions of Xe condensates in on-surface confinements induced by temperature changes and local probe excitation. The pores of a metal-organic network occupied with 1 up to 9 Xe atoms are investigated in their propensity to undergo "condensed solid" to "confined fluid" transitions. Different transition temperatures are identified, which depend on the number of Xe atoms in the condensate and relate to the stability of the Xe clustering in the condensed "phase." This work reveals the feature-rich behavior of transitions of confined planar condensates, which provide a showcase toward future "phase-transition" storage media patterned by self-assembly. This work is also of fundamental interest as it paves the way to real space investigations of reversible solid to fluid transitions of magic cluster condensates in an array of extremely well-defined quantum confinements.
The cover picture illustrates a novel concept for colorimetric protein sensing based on the controllable assembly of polypeptide-functionalized gold nanoparticles. Recognition of the analyte is accomplished by polypeptide-based synthetic receptors immobilized on gold nanoparticles. Also present on the particle surface is a de novo-designed helix-loop-helix polypeptide that homodimerizes and folds into four-helix bundles in the presence of Zn2+, resulting in particle aggregation. Analyte binding interferes with the folding-induced aggregation, giving rise to a clearly detectable colorimetric response.
Metal halide perovskites are multifunctional semiconductors with tunable structures and properties. They are highly dynamic crystals with complex octahedral tilting patterns and strongly anharmonic atomic behavior. In the higher temperature, higher symmetry phases of these materials, several complex structural features are observed. The local structure can differ greatly from the average structure and there is evidence that dynamic 2D structures of correlated octahedral motion form. An understanding of the underlying complex atomistic dynamics is, however, still lacking. In this work, the local structure of the inorganic perovskite CsPbI3 is investigated using a new machine learning force field based on the atomic cluster expansion framework. Through analysis of the temporal and spatial correlation observed during large-scale simulations, it is revealed that the low frequency motion of octahedral tilts implies a double-well effective potential landscape, even well into the cubic phase. Moreover, dynamic local regions of lower symmetry are present within both higher symmetry phases. These regions are planar and the length and timescales of the motion are reported. Finally, the spatial arrangement of these features and their interactions are investigated and visualized, providing a comprehensive picture of local structure in the higher symmetry phases.
Electronic control of biological processes with bioelectronic devices holds promise for sophisticated regulation of physiology, for gaining fundamental understanding of biological systems, providing new therapeutic solutions, and digitally mediating adaptations of organisms to external factors. The organic electronic ion pump (OEIP) provides a unique means for electronically-controlled, flow-free delivery of ions, and biomolecules at cellular scale. Here, a miniaturized OEIP device based on glass capillary fibers (c-OEIP) is implanted in a biological organism. The capillary form factor at the sub-100 mu m scale of the device enables it to be implanted in soft tissue, while its hyperbranched polyelectrolyte channel and addressing protocol allows efficient delivery of a large aromatic molecule. In the first example of an implantable bioelectronic device in plants, the c-OEIP readily penetrates the leaf of an intact tobacco plant with no significant wound response (evaluated up to 24 h) and effectively delivers the hormone abscisic acid (ABA) into the leaf apoplast. OEIP-mediated delivery of ABA, the phytohormone that regulates plants tolerance to stress, induces closure of stomata, the microscopic pores in leafs epidermis that play a vital role in photosynthesis and transpiration. Efficient and localized ABA delivery reveals previously unreported kinetics of ABA-induced signal propagation.
Nanoplatelets (NPLs) share excellent luminescent properties with their symmetric quantum dots counterparts and entail special characters benefiting from the shape, like the thickness-dependent bandgap and anisotropic luminescence. However, perovskite NPLs, especially those based on iodide, suffer from poor spectral and phase stability. Here, stable CsPbI3 NPLs obtained by accelerating the crystallization process in ambient-condition synthesis are reported. By this kinetic control, the rectangular NPLs into quasi-square NPLs are tuned, where enlarged width endows the NPLs with a lower surface-area-to-volume ratio (S/V ratio), leading to lower surficial energy and thus improved endurance against NPL fusion (cause for spectral shift or phase transformation). The accelerated crystallization, denoting the fast nucleation and short period of growth in this report, is enabled by preparing a precursor with complete transformation of PbI2 into intermediates (PbI3-), through an additional iodide supplier (e.g., zinc iodide). The excellent color stability of the materials remains in the light-emitting diodes under various bias stresses.
Semiconductor nanowires (NWs) are attracting increasing interest as nanobuilding blocks for optoelectronics and photonics. A novel material system that is highly suitable for these applications are GaNP NWs. In this article, we show that individual GaP/GaNP core/shell nanowires (NWs) grown by molecular beam epitaxy on Si substrates can act as Fabry-Perot (FP) microcavities. This conclusion is based on results of microphotoluminescence (μ-PL) measurements performed on individual NWs, which reveal periodic undulations of the PL intensity that follow an expected pattern of FP cavity modes. The cavity is concluded to be formed along the NW axis with the end facets acting as reflecting mirrors. The formation of the FP modes is shown to be facilitated by an increasing index contrast with the surrounding media. Spectral dependence of the group refractive index is also determined for the studied NWs. The observation of the FP microcavity modes in the GaP/GaNP core/shell NWs can be considered as a first step toward achieving lasing in this quasidirect bandgap semiconductor in the NW geometry.
Semiconductor nanowires (NWs) have recently gained increasing interest due to their great potential for photovoltaics. A novel material system based on GaNP NWs is considered to be highly suitable for applications in efficient multi-junction and intermediate band solar cells. This work shows that though the bandgap energies of GaNx P1-x alloys lie within the visible spectral range (i.e., within 540-650 nm for the currently achievable x < 3%), coaxial GaNP NWs grown on Si substrates can also harvest infrared light utilizing energy upconversion. This energy upconversion can be monitored via anti-Stokes near-band-edge photoluminescence (PL) from GaNP, visible even from a single NW. The dominant process responsible for this effect is identified as being due to two-step two-photon absorption (TS-TPA) via a deep level lying at about 1.28 eV above the valence band, based on the measured dependences of the anti-Stokes PL on excitation power and wavelength. The formation of the defect participating in the TS-TPA process is concluded to be promoted by nitrogen incorporation. The revealed defect-mediated TS-TPA process can boost efficiency of harvesting solar energy in GaNP NWs, beneficial for applications of this novel material system in third-generation photovoltaic devices.
The threshold voltage is an important property of organic field-effect transistors. By applying a self-assembled monolayer (SAM) on the gate dielectric, the value can be tuned. After electrical characterization, the semiconductor is delaminated. The surface potentials of the revealed SAM perfectly agree with the threshold voltages, which demonstrate that the shift is not due to the dipolar contribution, but due to charge trapping by the SAM.
In this study the fully acidic form of PEDOT-S was used for the purpose of self-assembly onto DNA. We have previously shown that PEDOT-S is a short polymer that is self-doped with !1/3 of the sulfonate side groups acting as the self-doping sites (see supporting info.). The remaining sulfonate groups contribute to a net anionic charge, and a water-soluble polymer, with an intrinsic bulk conductivity of around 30 S/cm. It has been shown that PEDOT-S can bind to oppositely charged cationic amyloid protein structures in water and form conducting nano fibrillar networks, and it has also been shown to form hybrid structures with synthetic peptides, and gold nanoparticles.
The development of high-efficiency, robust, and available electrode materials for oxygen evolution reaction (OER) and lithium-ion batteries (LIBs) is critical for clean and sustainable energy system but remains challenging. Herein, a unique yolk-shell structure of Fe2O3 nanotube@hollow Co9S8 nanocage@C is rationally prepared. In a prearranged sequence, the fabrication of Fe2O3 nanotubes is followed by coating of zeolitic imidazolate framework (ZIF-67) layer, chemical etching of ZIF-67 by thioacetamide, and eventual annealing treatment. Benefiting from the hollow structures of Fe2O3 nanotubes and Co9S8 nanocages, the conductivity of carbon coating and the synergy effects between different components, the titled sample possesses abundant accessible active sites, favorable electron transfer rate, and exceptional reaction kinetics in the electrocatalysis. As a result, excellent electrocatalytic activity for alkaline OER is achieved, which delivers a low overpotential of 205 mV at the current density of 10 mA cm(-2) along with the Tafel slope of 55 mV dec(-1). Moreover, this material exhibits excellent high-rate capability and excellent cycle life when employed as anode material of LIBs. This work provides a novel approach for the design and the construction of multifunctional electrode materials for energy conversion and storage.
Developing efficient and robust non-precious-metal-based catalysts to accelerate electrocatalytic reaction kinetics is crucial for electrochemical water-urea splitting. Herein, Fe-doped NiS-NiS2 heterostructured microspheres, an electrocatalyst, are synthesized via etching Prussian blue analogues following a controlled annealing treatment. The resulting microspheres are constructed by mesoporous nanoplates, granting the virtues of large surface areas, high structural void porosity, and accessible inner surface. These advantages not only provide more redox reaction centers but also strengthen structural robustness and effectively facilitate the mass diffusion and charge transport. Density functional theory simulations validate that the Fe-doping improves the conductivity of nickel sulfides, whereas the NiS-NiS2 heterojunctions induce interface charge rearrangement for optimizing the adsorption free energy of intermediates, resulting in a low overpotential and high electrocatalytic activity. Specifically, an ultralow overpotential of 270 mV at 50 mA cm(-2) for the oxygen evolution reaction (OER) is achieved. After adding 0.33 M urea into 1 M KOH, Fe-doped NiS-NiS2 obtains a strikingly reduced urea oxidation reaction potential of 1.36 V to reach 50 mA cm(-2), around 140 mV less than OER. This work provides insights into the synergistic modulation of electrocatalytic activity of non-noble catalysts for applications in energy conversion systems.
Vanadium dioxide (VO2) received tremendous interest lately due to its unique structural, electronic, and optoelectronic properties. VO2 has been extensively used in electrochromic displays and memristors and its VO2 (B) polymorph is extensively utilized as electrode material in energy storage applications. More studies are focused on VO2 (B) nanostructures which displayed different energy storage behavior than the bulk VO2. The present review provides a systematic overview of the progress in VO2 nanostructures syntheses and its application in energy storage devices. Herein, a general introduction, discussion about crystal structure, and syntheses of a variety of nanostructures such as nanowires, nanorods, nanobelts, nanotubes, carambola shaped, etc. are summarized. The energy storage application of VO2 nanostructure and its composites are also described in detail and categorically, e.g. Li-ion battery, Na-ion battery, and supercapacitors. The current status and challenges associated with VO2 nanostructures are reported. Finally, light has been shed for the overall performance improvement of VO2 nanostructure as potential electrode material for future application.
Endowing a semiconductor with tunable edge active sites will effectively enhance catalytic performance. Herein, an edge-site-rich ordered macroporous BiOCl (BiOCl-P) with abundant dangling bonds is constructed via the colloidal crystal template method. The edge-site-rich ordered macroporous structure provides abundant adsorption sites for CO2 molecules, as well as forms numerous localized electron enrichment areas, accelerating charge transfer. DFT calculations reveal that the dangling bonds-rich configuration can effectively reduce the CO2 activation energy barrier, boost the C(sic)O double bond dissociation, and facilitate the proton electron coupling reaction. As a result, the BiOCl-P achieves a higher CO and CH4 generation rate of 78.07 and 3.03 mu mol g(-1) under 4 h Xe lamp irradiation in a solid-gas system. Finally, the CO2 molecules conversion process is further investigated by in situ Fourier-transform infrared spectroscopy. This work realizes a new avenue toward the design of vibrant semiconductors on the nanoscale to boost inert CO2 photoreduction.
Shape-controlled synthesis of gold nanoparticles generally involves the use of surfactants, typically cetyltrimethylammonium (CTAX, X = Cl-, Br-), to regulate the nucleation growth process and to obtain colloidally stable nanoparticles. The surfactants adsorb on the nanoparticle surface making further functionalization difficult and therefore limit their use in many applications. Herein, the influence of CTAX on nanoparticle sensitivity to local dielectric environment changes is reported. It is shown, both experimentally and theoretically, that the CTAX bilayer significantly reduces the refractive index (RI) sensitivity of anisotropic gold nanoparticles such as nanocubes and concave nanocubes, nanorods, and nanoprisms. The RI sensitivity can be increased by up to 40% by removing the surfactant layer from nanoparticles immobilized on a solid substrate using oxygen plasma treatment. This increase compensates for the otherwise problematic decrease in RI sensitivity caused by the substrate effect. Moreover, the removal of the surfactants both facilitates nanoparticle biofunctionalization and significantly improves their catalytic properties. The strategy presented herein is a simple yet effective universal method for enhancing the RI sensitivity of CTAX-stabilized gold nanoparticles and increasing their potential as transducers in nanoplasmonic sensors, as well as in catalytic and biomedical applications.
A 2D array of electronically coupled quantum boxes is fabricated by means of on-surface self-assembly assuring ultimate precision of each box. The quantum states embedded in the boxes are configured by adsorbates, whose occupancy is controlled with atomic precision. The electronic interbox coupling can be maintained or significantly reduced by proper arrangement of empty and filled boxes.
Despite the remarkable advances made in the development of 2D perovskites suitable for various high-performance devices, the development of sub-30 nm nanopatterns of 2D perovskites with anisotropic photoelectronic properties remains challenging. Herein, a simple but robust route for fabricating sub-30 nm 1D nanopatterns of 2D perovskites over a large area is presented. This method is based on nanoimprinting a thin precursor film of a 2D perovskite with a topographically pre-patterned hard poly(dimethylsiloxane) mold replicated from a block copolymer nanopattern consisting of guided self-assembled monolayered in-plane cylinders. 1D nanopatterns of various 2D perovskites (A & PRIME;(2)MA(n)(-1)Pb(n)X(3)(n)(+1),A & PRIME; = BA, PEA, X = Br, I) are developed; their enhanced photoluminescence (PL) quantum yields are approximately four times greater than those of the corresponding control flat films. Anisotropic photocurrent is observed because 2D perovskite nanocrystals are embedded in a topological 1D nanopattern. Furthermore, this 1D metal-coated nanopattern of a 2D perovskite is employed as a color conversion optical polarizer, in which polarized PL is developed. This is due to its capability of polarization of an incident light arising from the sub-30 nm line pattern, as well as the PL of the confined 2D perovskite nanocrystals in the pattern.
Zinc oxide (ZnO) is a thermally stable n-type semiconducting material. ZnO 2D nanosheets have mainly gained substantial attention due to their unique properties, such as direct bandgap and strong excitonic binding energy at room temperature. These are widely utilized in piezotronics, energy storage, photodetectors, light-emitting diodes, solar cells, gas sensors, and photocatalysis. Notably, the chemical properties and performances of ZnO nanosheets largely depend on the nano-structuring that can be regulated and controlled through modulating synthetic strategies. Two synthetic approaches, top-down and bottom-up, are mainly employed for preparing ZnO 2D nanomaterials. However, owing to better results in producing defect-free nanostructures, homogenous chemical composition, etc., the bottom-up approach is extensively used compared to the top-down method for preparing ZnO 2D nanosheets. This review presents a comprehensive study on designing and developing 2D ZnO nanomaterials, followed by accenting its potential applications. To begin with, various synthetic strategies and attributes of ZnO 2D nanosheets are discussed, followed by focusing on methodologies and reaction mechanisms. Then, their deliberation toward batteries, supercapacitors, electronics/optoelectronics, photocatalysis, sensing, and piezoelectronic platforms are further discussed. Finally, the challenges and future opportunities are featured based on its current development.
The exploration of 2D solids is one of our times generators of materials discoveries. A recent addition to the 2D world is MXenes that possses a rich chemistry due to the large parent family of MAX phases. Recently, a new type of atomic laminated phases (coined i-MAX) is reported, in which two different transition metal atoms are ordered in the basal planes. Herein, these i-MAX phases are used in a new route for tailoriong the MXene structure and composition. By employing different etching protocols to the parent i-MAX phase (Mo2/3Y1/3)(2)AlC, the resulting MXene can be either: i) (Mo2/3Y1/3)(2)C with in-plane elemental order through selective removal of Al atoms or ii) Mo1.33C with ordered vacancies through selective removal of both Al and Y atoms. When (Mo2/3Y1/3)(2)C (ideal stoichiometry) is used as an electrode in a supercapacitor-with KOH electrolytea volumetric capacitance exceeding 1500 F cm(-3) is obtained, which is 40% higher than that of its Mo1.33C counterpart. With H2SO4, the trend is reversed, with the latter exhibiting the higher capacitance (approximate to 1200 F cm(-3)). This additional ability for structural tailoring will indubitably prove to be a powerful tool in property-tailoring of 2D materials, as exemplified here for supercapacitors.
Optical tweezers operated near solid-state membranes show unexplained periodic modulations in the optical trap position. An experimental study of the oscillations is presented, as well as optical simulations based on the finite-difference time-domain method, providing insight into the underlying interference phenomenon. This work provides a complete description as well as a solution to the enduring problem of modulations in optical traps near solid-state membranes.
Ionic thermoelectric materials can generate large thermal voltages under temperature gradients while also being low-cost and environmentally friendly. Many electrolytes with large Seebeck coefficients are reported in recent years, however, the mechanism of the thermal voltage is remained elusive. In this work, three types of polyelectrolytes are studied with different cations and identified a significant contribution to their thermal voltage originating from a concentration gradient. This conclusion is based on studies of the loss and gain of water upon temperature changes, variations in conductivity with water content and temperature, and the voltages induced by changes in water content. The results are analyzed by the "hopping mode" dynamics of charge transport in electrolytes. The hydration of different cations influences the water concentration gradient, which affects the barrier height and ion-induced potential in the electrodes. This work shows that the hydro-voltage in ionic thermoelectric devices can be one order of magnitude larger than the contribution from thermodiffusion-induced potentials, and becomes the main contributor to energy harvesting when implemented into ionic thermoelectric supercapacitors. Together with the rationalized theoretical discussion, this work clarifies the mechanism of thermal voltages in electrolytes and provides a new path for the development of ionic thermoelectric materials. The thermal voltage of polyelectrolyte films largely depends on the water concentration gradient under a temperature difference, which can be optimized to promote the generated total voltage up to over 30 mV K-1.image
For next-generation Internet-of-Everything applications, for example, artificial-neural-network image sensors, artificial retina, visible light communication, on-chip light interconnection, and flexible devices, etc., high-performance microscale photodetectors are in urgent demands. 2D material (2DM) photodetectors have been researched and demonstrated impressive performances. However, they have not met the demands in filterless narrowband photoresponse, wide linear dynamic range (LDR), ultralow dark current, and large on/off ratio, which are key performances for these applications. 2D Ruddlesden-Popper perovskites (2D-RPPs) are recently highlighted photovoltaic and optoelectronic materials. Embedding ultrathin 2D-RPPs into 2DM photodetectors holds potentials to improve these performances. Herein, a single-crystalline ultrathin (PEA)(2)PbI4 is integrated into a vertical-stacked graphene-(PEA)(2)PbI4-graphene micro photoconductor (V-PEPI-PC). V-PEPI-PC exhibits narrowband photoresponses at 517 nm with a full-width-at-half-maximum of 15 nm and a wide LDR of 122 dB. Due to the multiple quantum wells in (PEA)(2)PbI4, V-PEPI-PC demonstrates an ultralow dark current of 1.1 x 10(-14) A (44 pA mm(-2)), a high specific detectivity of 1.2 x 10(13) Jones, and a high on/off ratio of 1.6 x 10(6). Owing to the short vertical channel, V-PEPI-PC shows a fast response rise time of 486 mu s. Therefore, the vertical-stacked photodetectors based on hybrid 2D-RPPs and 2DMs may have great potentials in future optoelectronics.
Intrinsically stretchable multilayer circuit boards are fabricated with a fast and material efficient method based on filtration. Silver nanowire conductor patterns of outstanding performance are defined by filtration through wax printed membranes and the circuit board is assembled by subsequent transfers of the nanowires onto the elastomer substrate. The method is used to fabricate a bright stretchable light emitting diode matrix display.
Paper is emerging as a promising flexible, high surface-area substrate for various new applications such as printed electronics, energy storage, and paper-based diagnostics. Many applications, however, require paper that reaches metallic conductivity levels, ideally at low cost. Here, an aqueous electroless copper-plating method is presented, which forms a conducting thin film of fused copper nanoparticles on the surface of the cellulose fibers. This paper can be used as a current collector for anodes of lithium-ion batteries. Owing to the porous structure and the large surface area of cellulose fibers, the copper-plated paper-based half-cell of the lithium-ion battery exhibits excellent rate performance and cycling stability, and even outperforms commercially available planar copper foil-based anode at ultra-high charge/discharge rates of 100 C and 200 C. This mechanically robust metallic-paper composite has promising applications as the current collector for light-weight, flexible, and foldable paper-based 3D Li-ion battery anodes.
Chemodynamic therapy (CDT) is a highly targeted approach to treat cancer since it converts hydrogen peroxide into harmful hydroxyl radicals (OH & BULL;) through Fenton or Fenton-like reactions. However, the systemic toxicity of metal-based CDT agents has limited their clinical applications. Herein, a metal-free CDT agent: 2,4,6-tri(4-pyridyl)-1,3,5-triazine (TPT)/ [closo-B12H12]2-(TPT@ B12H12) is reported. Compared to the traditional metal-based CDT agents, TPT@B12H12 is free of metal avoiding cumulative toxicity during long-term therapy. Density functional theory (DFT) calculation revealed that TPT@B12H12 decreased the activation barrier more than 3.5 times being a more effective catalyst than the Fe2+ ion (the Fenton reaction), which decreases the barrier about twice. Mechanismly, the theory calculation indicated that both [B12H12]-& BULL; and [TPT-H]2+ have the capacity to decompose hydrogen into 1O2, OH & BULL;, and O2-& BULL;. With electron paramagnetic resonance and fluorescent probes, it is confirmed that TPT@B12H12 increases the levels of 1O2, OH & BULL;, and O2-& BULL;. More importantly, TPT@B12H12 effectively suppress the melanoma growth both in vitro and in vivo through 1O2, OH & BULL;, and O2-& BULL; generation. This study specifically highlights the great clinical translational potential of TPT@B12H12 as a CDT reagent. 2,4,6-Tri(4-pyridyl)-1,3,5-triazine (TPT)/ [closo-B12H12]2-(TPT@B12H12), a metal-free chemodynamic therapy (CDT) agent, decreases the activation barrier more than 3.5 times being a more effective catalyst than the Fe2+ ion (the Fenton reaction), which decreases the barrier about twice. More importantly, TPT@B12H12 effectively suppress the melanoma growth both in vitro and in vivo through 1O2, OH & BULL;, and O2-& BULL; generation. image
Molybdenum disulfide (MoS2 ), a typical layered 2D transition metal dichalcogenide, has received colossal interest in the past few years due to its unique structural, physicochemical, optical, and biological properties. While MoS2 is mostly applied in traditional industries such as dry lubricants, intercalation agents, and negative electrode material in lithium-ion batteries, its 2D and 0D forms have led to diverse applications in sensing, catalysis, therapy, and imaging. Herein, a systematic overview of the progress that is made in the field of MoS2 research with an emphasis on its different biomedical applications is presented. This article provides a general discussion on the basic structure and property of MoS2 and gives a detailed description of its different morphologies that are synthesized so far, namely, nanosheets, nanotubes, and quantum dots along with synthesis strategies. The biomedical applications of MoS2 -based nanocomposites are also described in detail and categorically, such as in varied therapeutic and diagnostic modalities like drug delivery, gene delivery, phototherapy, combined therapy, bioimaging, theranostics, and biosensing. Finally, a brief commentary on the current challenges and limitations being faced is provided, along with a discussion of some future perspectives for the overall improvement of MoS2 -based nanocomposites as a potential nanomedicine.
Semiconductor quantum dots (QDs) are among the most promising next-generation optoelectronic materials. QDs are generally obtained through either epitaxial or colloidal growth and carry the promise for solution-processed high-performance optoelectronic devices such as light-emitting diodes (LEDs), solar cells, etc. Herein, a straightforward approach to synthesize perovskite QDs and demonstrate their applications in efficient LEDs is reported. The perovskite QDs with controllable crystal sizes and properties are in situ synthesized through one-step spin-coating from perovskite precursor solutions followed by thermal annealing. These perovskite QDs feature size-dependent quantum confinement effect (with readily tunable emissions) and radiative monomolecular recombination. Despite the substantial structural inhomogeneity, the in situ generated perovskite QDs films emit narrow-bandwidth emission and high color stability due to efficient energy transfer between nanostructures that sweeps away the unfavorable disorder effects. Based on these materials, efficient LEDs with external quantum efficiencies up to 11.0% are realized. This makes the technologically appealing in situ approach promising for further development of state-of-the-art LED systems and other optoelectronic devices.
Given the breadth of currently arising opportunities and concerns associated with nanoparticles for biomedical imaging, various types of nanoparticles have been widely exploited, especially for cellular/subcellular level probing. However, most currently reported nanoparticles either have inefficient delivery into cells or lack specificity for intracellular destinations. The absence of well-defined nanoplatforms remains a critical challenge hindering practical nano-based bio-imaging. Herein, the authors elaborate on a tailorable membrane-penetrating nanoplatform as a carrier with encapsulated actives and decorated surfaces to tackle the above-mentioned issues. The tunable contents in such a versatile nanoplatform offer huge flexibility to reach the expected properties and functions. Aggregation-induced emission luminogen (AIEgen) is applied to achieve sought-after photophysical properties, specific targeting moieties are installed to give high affinity towards different desired organelles, and critical grafting of cell-penetrating cyclic disulfides (CPCDs) to promote cellular uptake efficiency without sacrificing the specificity. Hereafter, to validate its practicability, the tailored nano products are successfully applied to track the dynamic correlation between mitochondria and lysosomes during autophagy. The authors believe that the strategy and described materials can facilitate the development of functional nanomaterials for various life science applications.
Rational engineering of the surface properties of perovskite nanocrystals (PeNCs) is critical to obtain light emitters with simultaneous high photoluminescence efficiency and excellent charge transport properties for light-emitting diodes (LEDs). However, the commonly used lead halide sources make it hard to rationally optimize the surface compositions of the PeNCs. In addition, previously developed ligand engineering strategies for conventional inorganic nanocrystals easily deteriorate surface properties of the PeNCs, bringing additional difficulties in optimizing their optoelectronic properties. In this work, a novel strategy of employing a dual-purpose organic lead source for the synthesis of highly luminescent PeNCs with enhanced charge transport property is developed. Lead naphthenate (Pb(NA)(2)), of which the metal ions work as lead sources while the naphthenate can function as the surface ligands afterward, is explored and the obtained products under different synthesis conditions are comprehensively investigated. Monodispersed cesium lead bromide (CsPbBr3) with controllable size and excellent optical properties, showing superior photoluminescence quantum yields up to 80%, is obtained. Based on the simultaneously enhanced electrical properties of the Pb(NA)(2)-derived PeNCs, the resultant LEDs demonstrate a high peak external quantum efficiency of 8.44% and a superior maximum luminance of 31 759 cd cm(-2).
Abstract Using the MoS2-WTe2 heterostructure as a model system combined with electrochemical microreactors and density function theory calculations, it is shown that heterostructured contacts enhance the hydrogen evolution reaction (HER) activity of monolayer MoS2. Two possible mechanisms are suggested to explain this enhancement: efficient charge injection through large-area heterojunctions between MoS2 and WTe2 and effective screening of mirror charges due to the semimetallic nature of WTe2. The dielectric screening effect is proven minor, probed by measuring the HER activity of monolayer MoS2 on various support substrates with dielectric constants ranging from 4 to 300. Thus, the enhanced HER is attributed to the increased charge injection into MoS2 through large-area heterojunctions. Based on this understanding, a MoS2/WTe2 hybrid catalyst is fabricated with an HER overpotential of â140 mV at 10 mA cmâ2, a Tafel slope of 40 mV decâ1, and long stability. These results demonstrate the importance of interfacial design in transition metal dichalcogenide HER catalysts. The microreactor platform presents an unambiguous approach to probe interfacial effects in various electrocatalytic reactions.
A novel QD-molecule system is realized using metal–organic vapor-phase epitaxy growth. The dots are tunnel coupled via connected quantum wires (QWRs). The stronger tunnel coupling in this integrated QD-QWR system allows the hybridization of both electron and hole states, yielding direct-real-space excitonic molecules (see image). The structure holds promise for nanophotonic devices for quantum-information-processing applications.