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There have been many efforts to grow high-quality, single-crystalline graphene on a cheap substrate, such as a metal foil. However, control of nucleation and growth of individual flakes, as well as their seamless stitching, remains elusive. Here we demonstrate a new strategy to fast and facile synthesis of large scale single-crystal graphene on copper foil. Polycrystalline Cu foils were first converted to single-crystal Cu foils through high-temperature annealing processes. Then, a sodium chloride (NaCl) additive was introduced during chemical vapor deposition growth of graphene on the Cu foils. Investigation of early stage growth in this process suggests that the NaCl additive enhances nucleation events and depresses dendritic growth, producing high-density graphene flakes (GFs) with crystallographically well-defined edges: (i) rectangular-shaped GFs on Cu(100) and (ii) hexagonal-shaped GFs on Cu(111). Density functional theory calculations show that NaCl can assist in the elimination of remnant oxygen atoms on the Cu surface and promote epitaxial interactions between Cu and graphene. This behavior was further exploited to achieve large-scale single-crystal graphene through epitaxial, seamless stitching of hexagonal GFs within 90 s.

The synthesis of colloidal III-V quantum dots (QDs), particularly of the arsenides and antimonides, has been limited by the lack of stable and available group V precursors. In this work, we exploit accessible InCl

Colloidal nanorod heterostructures of I–III–VI2 semiconductors have been synthesized in a solution starting from wurtzite-like CuGaS2 nanorods. Growth of CuInS2 or CuInSe2 on CuGaS2 nanorods result...

Totally colorless, transparent, and highly refractive poly(phenylene thioether ether)s (PPTEs) containing thianthrene-2,7-disulfanyl moiety were developed in this study. A new 4,4′-diol aromatic compound, 2,7-(4,4′-diphenol)thiothianthrene (DPTT), with a high sulfur content was designed and synthesized to develop polymers with high refractive indices and high thermal stabilities. The PPTEs were prepared by polycondensation of DPTT with organic dihalogen compounds, such as 2,6-difluorobenzonitrile (DFBN) and 4,6-dichloro-2-(methylthio)pyrimidine (DCMP). The obtained polymers showed good thermal stabilities such as relatively high glass transition temperatures (Tgs) in the range of 153–176 °C and 5% weight loss temperatures (T5%) over 344 °C. The cut-off wavelengths (λ0) of the PPTE films are shorter than 343 nm, and they have a transmittance higher than 93% at 550 nm. The combination of the pyrimidine and high sulfur-containing thianthrene derivatives provides the PPTEs with a high refractive index of 1.7204 and a small birefringence of 0.0106 at 637 nm.

The analysis of circulating tumor cells (CTCs) in the peripheral blood of cancer patients is critical in clinical research for further investigation of tumor progression and metastasis. In this study, we present a novel surface-enhanced Raman scattering (SERS) substrate for the efficient capture and characterization of cancer cells using silver nanoparticles-reduced graphene oxide (AgNPs-rGO) composites. A pulsed laser reduction of silver nanowire-graphene oxide (AgNW-GO) mixture films induces hot-spot formations among AgNPs and artificial biointerfaces consisting of rGOs. We also use in situ electric field-assisted fabrication methods to enhance the roughness of the SERS substrate. The AgNW-GO mixture films, well suited for the proposed process due to its inherent electrophoretic motion, is adjusted between indium tin oxide (ITO) transparent electrodes and the nano-undulated surface is generated by applying direct-current (DC) electric fields during the laser process. As a result, MCF7 breast cancer cells are efficiently captured on the AgNPs-rGO substrates, about four times higher than the AgNWs-GO films, and the captured living cells are successfully analyzed by SERS spectroscopy. Our newly designed bifunctional substrate can be applied as an effective system for the capture and characterization of CTCs.

Li-iodine chemistry is of interest for electrochemical energy storage because it has been shown to provide both high power and high energy density. However, Li-iodine batteries are typically formed using Li metal and elemental iodine, which presents safety and fabrication challenges (e.g., the high vapor pressure of iodine). These disadvantages could be circumvented by using LiI as a starting cathode. Here, we present fabrication of a reduced graphene oxide (rGO)/LiI composite cathode, enabling for the first time the use of LiI as the Li-ion battery cathode. LiI was coated on rGO by infiltration of an ethanolic solution of LiI into a compressed rGO aerogel followed by drying. The free-standing rGO/LiI electrodes show stable long-term cycling and good rate performance with high specific capacity (200 mAh g–1 at 0.5 C after 100 cycles) and small hysteresis (0.056 V at 1 C). Shuttling was suppressed significantly. We speculate the improved electrochemical performance is due to strong interactions between the...

Anisotropic semiconductor nanoparticles find use in various applications ranging from electronics to photocatalysis and biolabeling. Batch synthesis methods typically used for their synthesis are often hampered by slow mixing, slow heating / cooling, and lack of batch-to-batch reproducibility, especially when scaling up. The modular continuous flow reactor reported here overcomes some of these challenges. It enables air-sensitive syntheses at temperatures as high as 400 °C, supports rapid heating and cooling times (~1 s or less), and enables syntheses that involve reagents that are viscous or even solid at room temperature. For validation we pursued two systems: the synthesis of (i) CdSe nanorods and bipods, and of (ii) ZnSe nanorods. Nanoparticles with low variance in quantum confined dimension (width) - 16% for CdSe and 11% for ZnSe - were obtained. For comparison, the same products were also synthesized using two batch approaches, hot-injection and heat-up, under similar conditions. The batch products were less uniform: 30% variance in quantum confined dimension. Furthermore, the lack of precise temperature control in the batch processes resulted in CdSe nanorods with irregular shaped, jagged branches whereas the continuous process produced CdSe nanorods with uniform, straight branches. The modular continuous flow reactor design is suited for scale up, allowing working flow rates as high as ~10 mL/min, which translates into a production rate of ~158 g / day for CdSe.

Colloidal quantum dots (QDs) are emerging as solution-processable, high-performance materials for light-emitting diodes (LEDs). Understanding the failure mechanism(s) is of both fundamental and practical importance, yet little is known of how QD-LEDs fail. Here, we have carried out accelerated device lifetime measurements on double heterojunction nanorod- (DHNR) and QD-LEDs. A common dependence of device lifetime on the initial driving voltage is observed over more than two orders of magnitude range in the initial luminance. This behavior is independent of whether the emitting materials are DHNRs or QDs prepared under different conditions. Reducing the hole injection barrier by doping HTL allows lower voltage operation, leading to longer device lifetimes. DHNRs with a band structure that further lowers the hole injection barrier require even lower driving voltages and therefore lead to longer device lifetimes than core/shell QDs. At 1000 cd m−2, the DHNR-LED exhibits no significant degradation even after more than 200 h of continuous operation. QD-LEDs, on the other hand, are completely degraded in less than ∼100 h under the same initial luminance conditions. Hole accumulation/trapping leading to HTL degradation, which in turn deteriorates electroluminescence but not the photoluminescence, is suggested to be the main cause of degradation of both DHNR- and QD-LEDs.

Colloidal semiconductor nanocrystals (NCs) are a promising materials class for solution-processable, next-generation electronic devices. However, most high-performance devices and circuits have bee...

The reliability of negative temperature coefficient (NTC) thermistors is one of the important factors for the excellent performance of the battery management system in electric vehicles. The electrical properties of the thermistor can be explained by the indirect electron jump between Mn3+ and Mn4+ at the B-sites in a spinel-type thermistor. Additionally, different types of dopants, such as Fe, Cu, Zn, Cr, and Mn, are considered as electrical modifiers that can further improve the electrical properties of the thermistor. For example, Cu is often added to NTC thermistors, occupying the octahedral sites in a spinel-type thermistor, which can play an important role in conduction with the Mn cations. Addition of Fe is also widely used in NTC thermistors owing to its high sensitivity, B constant, and stability. In this study, composition-dependent structural and electrical properties of Cu0.2/Fey-co-doped Ni0.3Mna-x-yCo0.9O4 (NMC) are investigated. Cu/Fe-co-doped NMC shows the R25 and B25/85 constant values of 4490–12730 Ω and 3185–3490 K, respectively, exhibiting a typical ρ–T curve of NTC thermistors. Higher B constant and reliable electrical stability are observed for Cu/Fe-co-doped NMC. Based on the relationship between the cationic oxidation states and electrical properties of Cu/Fe-co-doped NMC, the hopping conduction mechanism is discussed.

Crystal structures and hopping motions of cobalt manganese spinel oxides across a wide composition range (CoxMn3−xO4 (CMO), 0.9 ≤ x ≤ 2.7) are investigated in order to clarify the corresponding mechanisms of electrical behaviors as negative temperature coefficient thermistors. Based on the diffraction measurements, a tetragonal to cubic spinel transition are observed mostly with increasing Co content. Hopping distance for a series of CMO are calculated by the variable range hopping mechanism, which is changed as a function of composition, resulting to the observed unique electrical properties. According to the electrical and structural analysis, the electrical properties of CMO compounds with different Co contents majorly determined by tetragonal to cubic phase transition, cation distribution, and hopping distance. In addition, the formation of secondary phase (i.e., CoO) and another CMO phase may also significantly affect the electrical properties.

Size-tunable, narrow-bandwidth emission, low threshold voltage, and high external quantum efficiency (EQE) make quantum dot light-emitting diodes (QD-LEDs) promising in next-generation display and lighting technologies. However, the maximum efficiencies are often observed in a relatively low-current, low-brightness regime, and the efficiency droop leads to less-than-ideal performance at high-luminance conditions useful for many applications. Here, we examine solution-processed, double-heterojunction nanorod (DHNR)-LEDs with self-assembled monolayer (SAM) modified indium tin oxide (ITO) electrodes. The SAMs can modify the surface and the work function of ITO, facilitate hole transport into the device, and therefore improve charge balance in DHNR-LEDs. Extremely bright DHNR-LEDs with maximum luminance over 100 000 cd/m2 are demonstrated. Furthermore, maximum efficiencies appear at high luminance conditions that can be achieved at very low bias and current density (e.g., 3.1 V and 53 mA/cm2 at ∼10 000 cd/m2,...

Unexpected etching of nanocrystals, nanorods, and their heterostructures by one of the most commonly used metal precursors, metal oleates, is reported. Zn oleate is shown to etch CdS nanorods anisotropically, where the length decreases without a significant change in the diameter. Sodium oleate enhances the etch rate, whereas oleic acid alone does not cause etching, indicating the importance of the countercation on the rate of oleate induced etching. Subsequent addition of Se precursors to the partially etched nanorods in Zn oleate solution can lead to epitaxial growth of CdSe particles rather than the expected ZnSe growth, despite an excess amount of Zn precursors being present. The composition of this epitaxial growth can be varied from CdSe to ZnSe, depending on the amount of excess oleic acid or the reaction temperature. Similar tuning of composition can be observed when starting with collinear CdSe/CdS/CdSe rod/rod/rod heterostructures and spherical CdS (or CdSe/CdS core/shell) nanocrystals. Conversion of collinear rod/rod/rod structures to barbells and interesting rod growth from nearly spherical particles among other structures can also result due to the initial etching effect of metal oleates. These observations have important implications on our understanding of nanocrystal heterostructure synthesis and open up new routes to varying the composition and morphology of these materials.

Development of a cost-effective oxygen evolution reaction (OER) catalyst for hydrogen production from water has attracted the attention of scientists due to its potential to solve current environmental and energy issues, such as CO2 emissions and depletion of fossil fuels. In this paper, we report a facile synthesis to develop cobalt-manganese-oxide (MnxCo3−xO4, CMO) nanorods via an oxalate precipitation method followed by annealing at different temperatures. Importantly, morphology and surface area of the CMO nanorods, which are directly related to the OER activity, can be precisely controlled by changing annealing temperatures. The CMO nanorods engineered by oxalate precipitation and subsequent heat treatment show promising OER catalytic performance, such as a small overpotential of 365 mV for generating a current density of 10 mA cm−2, a low Tafel slope of 50.6 mV dec−1, and excellent long-term stability in alkaline media. Electrochemical properties combined with materials characterization provide insightful information on the OER mechanism of the CMO nanorods.

Recently developed approaches in deterministic assembly allow for controlled, geometric transformation of two-dimensional structures into complex, engineered three-dimensional layouts. Attractive features include applicability to wide ranging layout designs and dimensions along with the capacity to integrate planar thin film materials and device layouts. The work reported here establishes further capabilities for directly embedding high-performance electronic devices into the resultant 3D constructs based on silicon nanomembranes (Si NMs) as the active materials in custom devices or microscale components released from commercial wafer sources. Systematic experimental studies and theoretical analysis illustrate the key ideas through varied 3D architectures, from interconnected bridges and coils to extended chiral structures, each of which embed n-channel Si NM MOSFETs (nMOS), Si NM diodes, and p-channel silicon MOSFETs (pMOS). Examples in stretchable/deformable systems highlight additional features of these platforms. These strategies are immediately applicable to other wide-ranging classes of materials and device technologies that can be rendered in two-dimensional layouts, from systems for energy storage, to photovoltaics, optoelectronics, and others.

Dual-functioning displays, which can simultaneously transmit and receive information and energy through visible light, would enable enhanced user interfaces and device-to-device interactivity. We demonstrate that double heterojunctions designed into colloidal semiconductor nanorods allow both efficient photocurrent generation through a photovoltaic response and electroluminescence within a single device. These dual-functioning, all-solution-processed double-heterojunction nanorod light-responsive light-emitting diodes open feasible routes to a variety of advanced applications, from touchless interactive screens to energy harvesting and scavenging displays and massively parallel display-to-display data communication.

Here, we report multilayer stacking of films of quantum dots (QDs) for the purpose of tailoring the energy band alignment between charge transport layers and light emitting layers of different color in quantum dot light-emitting diodes (QD LED) for maximum efficiency in full color operation. The performance of QD LEDs formed by transfer printing compares favorably to that of conventional devices fabricated by spin-casting. Results indicate that zinc oxide (ZnO) and titanium dioxide (TiO2) can serve effectively as electron transport layers (ETLs) for red and green/blue QD LEDs, respectively. Optimized selections for each QD layer can be assembled at high yields by transfer printing with sacrificial fluoropolymer thin films to provide low energy surfaces for release, thereby allowing shared common layers for hole injection (HIL) and hole transport (HTL), along with customized ETLs. This strategy allows cointegration of devices with heterogeneous energy band diagrams, in a parallelized scheme that offers potential for high throughput and practical use.

A strategy of materials synthesis, characteristic evaluations, and manufacturing process for a mechanically elastic, biologically safe silicon-based dopamine detector that is designed to be completely transient, i.e., dissolved in water and/or biofluids, potentially in the brain after a desired period of operation, is introduced. Use of inexpensive, bioresorbable iron (Fe)-based nanoparticles (NPs) is one of the attractive choices for efficient catalytic oxidation of dopamine as an alternative for noble, nontransient platinum (Pt) nanoparticles, based on extensive studies of synthesized materials and catalytic reactions. Arrays of transient dopamine sensors validate electrochemical functionality to determine physiological levels of dopamine and to selectively sense dopamine in a variety of neurotransmitters, illuminating feasibilities for a higher level of soft, transient electronic implants integrated with other components of overall system.