scispace - formally typeset
Search or ask a question

Showing papers in "Nature Materials in 2004"


Journal ArticleDOI
TL;DR: This work is able to synthesize as much as 40 g of monodisperse nanocrystals in a single reaction, without a size-sorting process, and the particle size could be controlled simply by varying the experimental conditions.
Abstract: The development of nanocrystals has been intensively pursued, not only for their fundamental scientific interest, but also for many technological applications. The synthesis of monodisperse nanocrystals (size variation <5%) is of key importance, because the properties of these nanocrystals depend strongly on their dimensions. For example, the colour sharpness of semiconductor nanocrystal-based optical devices is strongly dependent on the uniformity of the nanocrystals, and monodisperse magnetic nanocrystals are critical for the next-generation multi-terabit magnetic storage media. For these monodisperse nanocrystals to be used, an economical mass-production method needs to be developed. Unfortunately, however, in most syntheses reported so far, only sub-gram quantities of monodisperse nanocrystals were produced. Uniform-sized nanocrystals of CdSe (refs 10,11) and Au (refs 12,13) have been produced using colloidal chemical synthetic procedures. In addition, monodisperse magnetic nanocrystals such as Fe (refs 14,15), Co (refs 16-18), gamma-Fe(2)O(3) (refs 19,20), and Fe(3)O(4) (refs 21,22) have been synthesized by using various synthetic methods. Here, we report on the ultra-large-scale synthesis of monodisperse nanocrystals using inexpensive and non-toxic metal salts as reactants. We were able to synthesize as much as 40 g of monodisperse nanocrystals in a single reaction, without a size-sorting process. Moreover, the particle size could be controlled simply by varying the experimental conditions. The current synthetic procedure is very general and nanocrystals of many transition metal oxides were successfully synthesized using a very similar procedure.

3,704 citations


Journal ArticleDOI
TL;DR: A giant MR ratio up to 180% at room temperature in single-crystal Fe/MgO/Fe MTJs is reported, indicating that coherency of wave functions is conserved across the tunnel barrier.
Abstract: The tunnel magnetoresistance (TMR) effect in magnetic tunnel junctions (MTJs)1,2 is the key to developing magnetoresistive random-access-memory (MRAM), magnetic sensors and novel programmable logic devices3,4,5. Conventional MTJs with an amorphous aluminium oxide tunnel barrier, which have been extensively studied for device applications, exhibit a magnetoresistance ratio up to 70% at room temperature6. This low magnetoresistance seriously limits the feasibility of spintronics devices. Here, we report a giant MR ratio up to 180% at room temperature in single-crystal Fe/MgO/Fe MTJs. The origin of this enormous TMR effect is coherent spin-polarized tunnelling, where the symmetry of electron wave functions plays an important role. Moreover, we observed that their tunnel magnetoresistance oscillates as a function of tunnel barrier thickness, indicating that coherency of wave functions is conserved across the tunnel barrier. The coherent TMR effect is a key to making spintronic devices with novel quantum-mechanical functions, and to developing gigabit-scale MRAM.

2,956 citations


Journal ArticleDOI
TL;DR: Sputter-deposited polycrystalline MTJs grown on an amorphous underlayer, but with highly oriented MgO tunnel barriers and CoFe electrodes, exhibit TMR values of up to ∼220% at room temperature and ∼300% at low temperatures, which will accelerate the development of new families of spintronic devices.
Abstract: Magnetically engineered magnetic tunnel junctions (MTJs) show promise as non-volatile storage cells in high-performance solid-state magnetic random access memories (MRAM). The performance of these devices is currently limited by the modest (< approximately 70%) room-temperature tunnelling magnetoresistance (TMR) of technologically relevant MTJs. Much higher TMR values have been theoretically predicted for perfectly ordered (100) oriented single-crystalline Fe/MgO/Fe MTJs. Here we show that sputter-deposited polycrystalline MTJs grown on an amorphous underlayer, but with highly oriented (100) MgO tunnel barriers and CoFe electrodes, exhibit TMR values of up to approximately 220% at room temperature and approximately 300% at low temperatures. Consistent with these high TMR values, superconducting tunnelling spectroscopy experiments indicate that the tunnelling current has a very high spin polarization of approximately 85%, which rivals that previously observed only using half-metallic ferromagnets. Such high values of spin polarization and TMR in readily manufactureable and highly thermally stable devices (up to 400 degrees C) will accelerate the development of new families of spintronic devices.

2,931 citations


Journal ArticleDOI
TL;DR: HBN is shown to be a promising material for compact ultraviolet laser devices because it has a direct bandgap in the ultraviolet region and evidence for room-temperature ultraviolet lasing at 215 nm by accelerated electron excitation is provided.
Abstract: The demand for compact ultraviolet laser devices is increasing, as they are essential in applications such as optical storage, photocatalysis, sterilization, ophthalmic surgery and nanosurgery. Many researchers are devoting considerable effort to finding materials with larger bandgaps than that of GaN. Here we show that hexagonal boron nitride (hBN) is a promising material for such laser devices because it has a direct bandgap in the ultraviolet region. We obtained a pure hBN single crystal under high-pressure and high-temperature conditions, which shows a dominant luminescence peak and a series of s-like exciton absorption bands around 215 nm, proving it to be a direct-bandgap material. Evidence for room-temperature ultraviolet lasing at 215 nm by accelerated electron excitation is provided by the enhancement and narrowing of the longitudinal mode, threshold behaviour of the excitation current dependence of the emission intensity, and a far-field pattern of the transverse mode.

2,550 citations


Journal ArticleDOI
TL;DR: In this paper, the authors used a new technique to fabricate p-type ZnO reproducibly, and showed high-quality undoped films with electron mobility exceeding that in the bulk.
Abstract: Since the successful demonstration of a blue light-emitting diode (LED)1, potential materials for making short-wavelength LEDs and diode lasers have been attracting increasing interest as the demands for display, illumination and information storage grow2,3,4. Zinc oxide has substantial advantages including large exciton binding energy, as demonstrated by efficient excitonic lasing on optical excitation5,6. Several groups have postulated the use of p-type ZnO doped with nitrogen, arsenic or phosphorus7,8,9,10, and even p–n junctions11,12,13. However, the choice of dopant and growth technique remains controversial and the reliability of p-type ZnO is still under debate14. If ZnO is ever to produce long-lasting and robust devices, the quality of epitaxial layers has to be improved as has been the protocol in other compound semiconductors15. Here we report high-quality undoped films with electron mobility exceeding that in the bulk. We have used a new technique to fabricate p-type ZnO reproducibly. Violet electroluminescence from homostructural p–i–n junctions is demonstrated at room-temperature.

1,964 citations


Journal ArticleDOI
TL;DR: Flexible active-matrix monochrome electrophoretic displays based on solution-processed organic transistors on 25-μm-thick polyimide substrates based on 1,888 transistors are demonstrated, which are the largest organic integrated circuits reported to date.
Abstract: At present, flexible displays are an important focus of research1,2,3 Further development of large, flexible displays requires a cost-effective manufacturing process for the active-matrix backplane, which contains one transistor per pixel One way to further reduce costs is to integrate (part of) the display drive circuitry, such as row shift registers, directly on the display substrate Here, we demonstrate flexible active-matrix monochrome electrophoretic displays based on solution-processed organic transistors on 25-μm-thick polyimide substrates The displays can be bent to a radius of 1 cm without significant loss in performance Using the same process flow we prepared row shift registers With 1,888 transistors, these are the largest organic integrated circuits reported to date More importantly, the operating frequency of 5 kHz is sufficiently high to allow integration with the display operating at video speed This work therefore represents a major step towards 'system-on-plastic'

1,577 citations


Journal ArticleDOI
TL;DR: The discovery that the extract from the lemongrass plant, when reacted with aqueous chloroaurate ions, yields a high percentage of thin, flat, single-crystalline gold nanotriangles, which seem to grow by a process involving rapid reduction, assembly and room-temperature sintering of 'liquid-like' spherical gold nanoparticles.
Abstract: The optoelectronic and physicochemical properties of nanoscale matter are a strong function of particle size. Nanoparticle shape also contributes significantly to modulating their electronic properties. Several shapes ranging from rods to wires to plates to teardrop structures may be obtained by chemical methods; triangular nanoparticles have been synthesized by using a seeded growth process. Here, we report the discovery that the extract from the lemongrass plant, when reacted with aqueous chloroaurate ions, yields a high percentage of thin, flat, single-crystalline gold nanotriangles. The nanotriangles seem to grow by a process involving rapid reduction, assembly and room-temperature sintering of 'liquid-like' spherical gold nanoparticles. The anisotropy in nanoparticle shape results in large near-infrared absorption by the particles, and highly anisotropic electron transport in films of the nanotriangles.

1,473 citations


Journal ArticleDOI
TL;DR: The results indicate that the use of SPs would lead to a new class of very bright LEDs, and highly efficient solid-state light sources.
Abstract: Since 1993, InGaN light-emitting diodes (LEDs) have been improved and commercialized, but these devices have not fulfilled their original promise as solid-state replacements for light bulbs as their light-emission efficiencies have been limited. Here we describe a method to enhance this efficiency through the energy transfer between quantum wells (QWs) and surface plasmons (SPs). SPs can increase the density of states and the spontaneous emission rate in the semiconductor, and lead to the enhancement of light emission by SP–QW coupling. Large enhancements of the internal quantum efficiencies (etaint) were measured when silver or aluminium layers were deposited 10 nm above an InGaN light-emitting layer, whereas no such enhancements were obtained from gold-coated samples. Our results indicate that the use of SPs would lead to a new class of very bright LEDs, and highly efficient solid-state light sources.

1,349 citations


Journal ArticleDOI
TL;DR: Recent developments of SOFC fuel electrodes that will enable the better use of readily available fuels are discussed, particularly the fuel electrode or anode.
Abstract: Fuel cells will undoubtedly find widespread use in this new millennium in the conversion of chemical to electrical energy, as they offer very high efficiencies and have unique scalability in electricity-generation applications. The solid-oxide fuel cell (SOFC) is one of the most exciting of these energy technologies; it is an all-ceramic device that operates at temperatures in the range 500–1,000 °C. The SOFC offers certain advantages over lower temperature fuel cells, notably its ability to use carbon monoxide as a fuel rather than being poisoned by it, and the availability of high-grade exhaust heat for combined heat and power, or combined cycle gas-turbine applications. Although cost is clearly the most important barrier to widespread SOFC implementation, perhaps the most important technical barriers currently being addressed relate to the electrodes, particularly the fuel electrode or anode. In terms of mitigating global warming, the ability of the SOFC to use commonly available fuels at high efficiency, promises an effective and early reduction in carbon dioxide emissions, and hence is one of the lead new technologies for improving the environment. Here, we discuss recent developments of SOFC fuel electrodes that will enable the better use of readily available fuels.

1,332 citations


Journal ArticleDOI
TL;DR: An elegant, efficient measurement method that yields the elastic moduli of nanoscale polymer films in a rapid and quantitative manner without the need for expensive equipment or material-specific modelling is introduced.
Abstract: As technology continues towards smaller, thinner and lighter devices, more stringent demands are placed on thin polymer films as diffusion barriers, dielectric coatings, electronic packaging and so on. Therefore, there is a growing need for testing platforms to rapidly determine the mechanical properties of thin polymer films and coatings. We introduce here an elegant, efficient measurement method that yields the elastic moduli of nanoscale polymer films in a rapid and quantitative manner without the need for expensive equipment or material-specific modelling. The technique exploits a buckling instability that occurs in bilayers consisting of a stiff, thin film coated onto a relatively soft, thick substrate. Using the spacing of these highly periodic wrinkles, we calculate the film's elastic modulus by applying well-established buckling mechanics. We successfully apply this new measurement platform to several systems displaying a wide range of thicknessess (nanometre to micrometre) and moduli (MPa to GPa).

1,264 citations


Journal ArticleDOI
TL;DR: New concepts and principles of using severe plastic deformation to fabricate bulk nanostructured metals with advanced properties are discussed, with special emphasis on the relationship between microstructural features and properties, as well as the first applications of SPD-produced nanomaterials.
Abstract: Despite rosy prospects, the use of nanostructured metals and alloys as advanced structural and functional materials has remained controversial until recently. Only in recent years has a breakthrough been outlined in this area, associated both with development of new routes for the fabrication of bulk nanostructured materials and with investigation of the fundamental mechanisms that lead to the new properties of these materials. Although a deep understanding of these mechanisms is still a topic of basic research, pilot commercial products for medicine and microdevices are coming within reach of the market. This progress article discusses new concepts and principles of using severe plastic deformation (SPD) to fabricate bulk nanostructured metals with advanced properties. Special emphasis is laid on the relationship between microstructural features and properties, as well as the first applications of SPD-produced nanomaterials.

Journal ArticleDOI
TL;DR: It is demonstrated that, different from the current consensus, Ge2Sb2Te5, the material of choice in DVD-RAM, does not possess the rocksalt structure but more likely consists of well-defined rigid building blocks that are randomly oriented in space consistent with cubic symmetry.
Abstract: Present-day multimedia strongly rely on rewritable phase-change optical memories. We demonstrate that, different from the current consensus, Ge(2)Sb(2)Te(5), the material of choice in DVD-RAM, does not possess the rocksalt structure but more likely consists of well-defined rigid building blocks that are randomly oriented in space consistent with cubic symmetry. Laser-induced amorphization results in drastic shortening of covalent bonds and a decrease in the mean-square relative displacement, demonstrating a substantial increase in the degree of short-range ordering, in sharp contrast to the amorphization of typical covalently bonded solids. This novel order-disorder transition is due to an umbrella-flip of Ge atoms from an octahedral position into a tetrahedral position without rupture of strong covalent bonds. It is this unique two-state nature of the transformation that ensures fast DVD performance and repeatable switching over ten million cycles.

Journal ArticleDOI
TL;DR: In this article, the first compelling atomic structural model for metallic glasses is presented, which is based on a new sphere-packing scheme and combines random positioning of solvent atoms and medium-range atomic order of solute atoms.
Abstract: Despite the intense interest in metallic glasses for a variety of engineering applications, many details of their structure remain a mystery. Here, we present the first compelling atomic structural model for metallic glasses. This structural model is based on a new sphere-packing scheme—the dense packing of atomic clusters. Random positioning of solvent atoms and medium-range atomic order of solute atoms are combined to reproduce diffraction data successfully over radial distances up to ∼1 nm. Although metallic glasses can have any number of chemically distinct solute species, this model shows that they contain no more than three topologically distinct solutes and that these solutes have specific and predictable sizes relative to the solvent atoms. Finally, this model includes defects that provide richness to the structural description of metallic glasses. The model accurately predicts the number of solute atoms in the first coordination shell of a typical solvent atom, and provides a remarkable ability to predict metallic-glass compositions accurately for a wide range of simple and complex alloys.

Journal ArticleDOI
TL;DR: This work demonstrates a simple and industrially scaleable route that yields a 1.5–5-fold improvement in the in-magnetic-field current densities of conductors that are already of high quality.
Abstract: There are numerous potential applications for superconducting tapes based on YBa(2)Cu(3)O(7-x) (YBCO) films coated onto metallic substrates. A long-established goal of more than 15 years has been to understand the magnetic-flux pinning mechanisms that allow films to maintain high current densities out to high magnetic fields. In fact, films carry one to two orders of magnitude higher current densities than any other form of the material. For this reason, the idea of further improving pinning has received little attention. Now that commercialization of YBCO-tape conductors is much closer, an important goal for both better performance and lower fabrication costs is to achieve enhanced pinning in a practical way. In this work, we demonstrate a simple and industrially scaleable route that yields a 1.5-5-fold improvement in the in-magnetic-field current densities of conductors that are already of high quality.

Journal ArticleDOI
TL;DR: The fabrication—through direct laser writing—and detailed characterization of high-quality large-scale f.c. c.
Abstract: The past decade has witnessed intensive research efforts related to the design and fabrication of photonic crystals1,2. These periodically structured dielectric materials can represent the optical analogue of semiconductor crystals, and provide a novel platform for the realization of integrated photonics. Despite intensive efforts, inexpensive fabrication techniques for large-scale three-dimensional photonic crystals of high enough quality, with photonic bandgaps at near-infrared frequencies, and built-in functional elements for telecommunication applications, have been elusive. Direct laser writing by multiphoton polymerization3 of a photoresist has emerged as a technique for the rapid, cheap and flexible fabrication of nanostructures for photonics. In 1999, so-called layer-by-layer4 or woodpile photonic crystals were fabricated with a fundamental stop band at 3.9 μm wavelength5. In 2002, a corresponding 1.9 μm was achieved6, but the important face-centred-cubic (f.c.c.) symmetry was abandoned. Importantly, fundamental stop bands or photonic bandgaps at telecommunication wavelengths have not been demonstrated. In this letter, we report the fabrication—through direct laser writing—and detailed characterization of high-quality large-scale f.c.c. layer-by-layer structures, with fundamental stop bands ranging from 1.3 to 1.7 μm.

Journal ArticleDOI
TL;DR: This work identifies the nature of the ferroelectric phase transition in the hexagonal manganite, YMnO3, using a combination of single-crystal X-ray diffraction, thorough structure analysis and first-principles density-functional calculations, and suggests an avenue for designing novel magnetic ferroelectrics.
Abstract: Understanding the ferroelectrocity in magnetic ferroelectric oxides is of both fundamental and technological importance. Here, we identify the nature of the ferroelectric phase transition in the hexagonal manganite, YMnO3, using a combination of single-crystal X-ray diffraction, thorough structure analysis and first-principles density-functional calculations. The ferroelectric phase is characterized by a buckling of the layered MnO5 polyhedra, accompanied by displacements of the Y ions, which lead to a net electric polarization. Our calculations show that the mechanism is driven entirely by electrostatic and size effects, rather than the usual changes in chemical bonding associated with ferroelectric phase transitions in perovskite oxides. As a result, the usual indicators of structural instability, such as anomalies in Born effective charges on the active ions, do not hold. In contrast to the chemically stabilized ferroelectrics, this mechanism for ferroelectricity permits the coexistence of magnetism and ferroelectricity, and so suggests an avenue for designing novel magnetic ferroelectrics.

Journal ArticleDOI
TL;DR: The demonstration of non-carbonaceous-network grain-boundary conduction to be the first in these materials, and that it holds promise for other insulating phosphates.
Abstract: The provision of efficient electron and ion transport is a critical issue in an exciting new group of materials based on lithium metal phosphates that are important as cathodes for lithium-ion batteries. Much interest centres on olivine-type LiFePO(4), the most prominent member of this family. Whereas the one-dimensional lithium-ion mobility in this framework is high, the electronically insulating phosphate groups that benefit the voltage also isolate the redox centres within the lattice. The pristine compound is a very poor conductor (sigma approximately 10(-9) S cm(-1)), thus limiting its electrochemical response. One approach to overcome this is to include conductive phases, increasing its capacity to near-theoretical values. There have also been attempts to alter the inherent conductivity of the lattice by doping it with a supervalent ion. Compositions were reported to be black p-type semiconductors with conductivities of approximately 10(-2) S cm(-1) arising from minority Fe(3+) hole carriers. Our results for doped (and undoped) LiMPO(4) (M = Fe, Ni) show that a percolating nano-network of metal-rich phosphides are responsible for the enhanced conductivity. We believe our demonstration of non-carbonaceous-network grain-boundary conduction to be the first in these materials, and that it holds promise for other insulating phosphates.

Journal ArticleDOI
TL;DR: Density functional theory calculations are used to introduce a new class of near-surface alloys that can yield superior catalytic behaviour for hydrogen-related reactions and may permit these alloys to serve as low-temperature, highly selective catalysts for pharmaceuticals production and as robust fuel-cell anodes.
Abstract: The rational design of pure and alloy metal catalysts from fundamental principles has the potential to yield catalysts of greatly improved activity and selectivity. A promising area of research concerns the role that near-surface alloys (NSAs) can play in endowing surfaces with novel catalytic properties. NSAs are defined as alloys wherein a solute metal is present near the surface of a host metal in concentrations different from the bulk; here we use density functional theory calculations to introduce a new class of these alloys that can yield superior catalytic behaviour for hydrogen-related reactions. Some of these NSAs bind atomic hydrogen (H) as weakly as the noble metals (Cu, Au) while, at the same time, dissociating H2 much more easily. This unique set of properties may permit these alloys to serve as low-temperature, highly selective catalysts for pharmaceuticals production and as robust fuel-cell anodes.

Journal ArticleDOI
TL;DR: It is shown that with a different mechanism, an aged BaTiO3 single crystal can generate a large recoverable nonlinear strain of 0.75% at a low field of 200 V mm−1.
Abstract: Large electric-field-induced strain in ferroelectric crystals by point-defect-mediated reversible domain switching

Journal ArticleDOI
TL;DR: This work demonstrates that the uniform dispersion of 1–5 vol.% of carbon nanotubes in a thermoplastic elastomer yields nanocomposites that can store and subsequently release, through remote means, up to 50% more recovery stress than the pristine resin.
Abstract: Stimuli-responsive (active) materials undergo large-scale shape or property changes in response to an external stimulus such as stress, temperature, light or pH1,2. Technological uses range from durable, shape-recovery eye-glass frames, to temperature-sensitive switches, to the generation of stress to induce mechanical motion3,4,5,6,7,8,9. Here, we demonstrate that the uniform dispersion of 1–5 vol.% of carbon nanotubes in a thermoplastic elastomer yields nanocomposites that can store and subsequently release, through remote means, up to 50% more recovery stress than the pristine resin. The anisotropic nanotubes increase the rubbery modulus by a factor of 2 to 5 (for 1–5 vol.%) and improve shape fixity by enhancing strain-induced crystallization. Non-radiative decay of infrared photons absorbed by the nanotubes raises the internal temperature, melting strain-induced polymer crystallites (which act as physical crosslinks that secure the deformed shape) and remotely trigger the release of the stored strain energy. Comparable effects occur for electrically induced actuation associated with Joule heating of the matrix when a current is passed through the conductive percolative network of the nanotubes within the resin. This unique combination of properties, directly arising from the nanocomposite morphology, demonstrates new opportunities for the design and fabrication of stimuli-responsive polymers, which are otherwise not available in one material system.

Journal ArticleDOI
TL;DR: The synthesis and successful testing of solution-phase, near-infrared sensors, with β-D-glucose sensing as a model system, using single-walled carbon nanotubes that modulate their emission in response to the adsorption of specific biomolecules are reported.
Abstract: Molecular detection using near-infrared light between 0.9 and 1.3 eV has important biomedical applications because of greater tissue penetration and reduced auto-fluorescent background in thick tissue or whole-blood media. Carbon nanotubes have a tunable near-infrared emission that responds to changes in the local dielectric function but remains stable to permanent photobleaching. In this work, we report the synthesis and successful testing of solution-phase, near-infrared sensors, with beta-D-glucose sensing as a model system, using single-walled carbon nanotubes that modulate their emission in response to the adsorption of specific biomolecules. New types of non-covalent functionalization using electron-withdrawing molecules are shown to provide sites for transferring electrons in and out of the nanotube. We also show two distinct mechanisms of signal transduction-fluorescence quenching and charge transfer. The results demonstrate new opportunities for nanoparticle optical sensors that operate in strongly absorbing media of relevance to medicine or biology.

Journal ArticleDOI
TL;DR: It is demonstrated here that by dissolving—rather than covalently bonding—azo dyes into an LCE sample, its mechanical deformation in response to non-uniform illumination by visible light becomes very large and is more than two orders of magnitude faster than previously reported.
Abstract: Liquid-crystal elastomers (LCEs) are rubbers whose constituent molecules are orientationally ordered. Their salient feature is strong coupling between the orientational order and mechanical strain. For example, changing the orientational order gives rise to internal stresses, which lead to strains and change the shape of a sample. Orientational order can be affected by changes in externally applied stimuli such as light. We demonstrate here that by dissolving-rather than covalently bonding-azo dyes into an LCE sample, its mechanical deformation in response to non-uniform illumination by visible light becomes very large (more than 60 degrees bending) and is more than two orders of magnitude faster than previously reported. Rapid light-induced deformations allow LCEs to interact with their environment in new and unexpected ways. When light from above is shone on a dye-doped LCE sample floating on water, the LCE 'swims' away from the light, with an action resembling that of flatfish such as skates or rays. We analyse the propulsion mechanism in terms of momentum transfer.

Journal ArticleDOI
TL;DR: It is shown, using molecular dynamics simulations, that the nature of slip in nanocrystalline metals cannot be described in terms of the absolute value of the stacking fault energy—a correct interpretation requires the generalized stacking faultEnergy curve, involving both stable and unstable stacking fault energies.
Abstract: The search for deformation mechanisms in nanocrystalline metals has profited from the use of molecular dynamics calculations. These simulations have revealed two possible mechanisms; grain boundary accommodation, and intragranular slip involving dislocation emission and absorption at grain boundaries. But the precise nature of the slip mechanism is the subject of considerable debate, and the limitations of the simulation technique need to be taken into consideration. Here we show, using molecular dynamics simulations, that the nature of slip in nanocrystalline metals cannot be described in terms of the absolute value of the stacking fault energy-a correct interpretation requires the generalized stacking fault energy curve, involving both stable and unstable stacking fault energies. The molecular dynamics technique does not at present allow for the determination of rate-limiting processes, so the use of our calculations in the interpretation of experiments has to be undertaken with care.

Journal ArticleDOI
TL;DR: A novel organic memory device fabricated by solution processing that displays an abrupt transition to a high-conductivity state under an external bias of 2.8 V and is non-volatile, indicating that the device may be used for low-cost, high-density memory storage.
Abstract: Building on the success of organic electronic devices, such as light-emitting diodes and field-effect transistors, procedures for fabricating non-volatile organic memory devices are now being explored. Here, we demonstrate a novel organic memory device fabricated by solution processing. Programmable electrical bistability was observed in a device made from a polystyrene film containing gold nanoparticles and 8-hydroxyquinoline sandwiched between two metal electrodes. The as-prepared device, which is in a low-conductivity state, displays an abrupt transition to a high-conductivity state under an external bias of 2.8 V. These two states differ in conductivity by about four orders of magnitude. Applying a negative bias of 1.8 V causes the device to return to the low-conductivity state. The electronic transition is attributed to the electric-field-induced charge transfer between the gold nanoparticles and 8-hydroxyquinoline. The transition from the low- to the high-conductivity state takes place in nanoseconds, and is non-volatile, indicating that the device may be used for low-cost, high-density memory storage.

Journal ArticleDOI
TL;DR: A new technique is discussed that enables us to control the charge density in the channel by using organosilane self-assembled monolayers (SAMs) on SiO2 gate insulators.
Abstract: Organic thin-film transistors are attracting a great deal of attention due to the relatively high field-effect mobility in several organic materials. In these organic semiconductors, however, researchers have not established a reliable method of doping at a very low density level, although this has been crucial for the technological development of inorganic semiconductors. In the field-effect device structures, the conduction channel exists at the interface between organic thin films and SiO2 gate insulators. Here, we discuss a new technique that enables us to control the charge density in the channel by using organosilane self-assembled monolayers (SAMs) on SiO2 gate insulators. SAMs with fluorine and amino groups have been shown to accumulate holes and electrons, respectively, in the transistor channel: these properties are understood in terms of the effects of electric dipoles of the SAMs molecules, and weak charge transfer between organic films and SAMs.

Journal ArticleDOI
TL;DR: This work has developed ABA block copolymeric amphiphiles that self-assemble into unilamellar vesicles that can be further oxidatively destabilized, the first example of the use of oxidative conversions to destabilize such carriers.
Abstract: Vesicles formed in water by synthetic macro-amphiphiles have attracted much attention as nanocontainers having properties that extend the physical and chemical limits of liposomes. We sought to develop ABA block copolymeric amphiphiles that self-assemble into unilamellar vesicles that can be further oxidatively destabilized. We selected poly(ethylene glycol) (PEG) as the hydrophilic A blocks, owing to its resistance to protein adsorption and low toxicity. As hydrophobic B blocks, we selected poly(propylene sulphide) (PPS), owing to its extreme hydrophobicity, its low glass-transition temperature, and most importantly its oxidative conversion from a hydrophobe to a hydrophile, poly(propylene sulphoxide) and ultimately poly(propylene sulphone). This is the first example of the use of oxidative conversions to destabilize such carriers. This new class of oxidation-responsive polymeric vesicles may find applications as nanocontainers in drug delivery, biosensing and biodetection.

Journal ArticleDOI
TL;DR: If all-optical devices using photonic crystal designs promise to be smaller than the wavelength of light, and to operate with bandwidths that are very difficult to achieve electronically, operation at single-photon power levels could be feasible.
Abstract: The quest for all-optical signal processing is generally deemed to be impractical because optical nonlinearities are usually weak. The emerging field of nonlinear photonic crystals seems destined to change this view dramatically. Theoretical considerations show that all-optical devices using photonic crystal designs promise to be smaller than the wavelength of light, and to operate with bandwidths that are very difficult to achieve electronically. When created in commonly used materials, these devices could operate at powers of only a few milliwatts. Moreover, if these designs are combined with materials and systems that support electromagnetically induced transparency, operation at single-photon power levels could be feasible.

Journal ArticleDOI
TL;DR: This method for immobilizing biomolecules in 3D matrices can generally be applied to any optically clear hydrogel, offering a solution to construct scaffolds with programmed spatial features for tissue engineering applications.
Abstract: Tissue engineering aims to replace, repair or regenerate tissue/organ function, by delivering signalling molecules and cells on a three-dimensional (3D) biomaterials scaffold that supports cell infiltration and tissue organization. To control cell behaviour and ultimately induce structural and functional tissue formation on surfaces, planar substrates have been patterned with adhesion signals that mimic the spatial cues to guide cell attachment and function. The objective of this study is to create biochemical channels in 3D hydrogel matrices for guided axonal growth. An agarose hydrogel modified with a cysteine compound containing a sulphydryl protecting group provides a photolabile substrate that can be patterned with biochemical cues. In this transparent hydrogel we immobilized the adhesive fibronectin peptide fragment, glycine-arginine-glycine-aspartic acid-serine (GRGDS), in selected volumes of the matrix using a focused laser. We verified in vitro the guidance effects of GRGDS oligopeptide-modified channels on the 3D cell migration and neurite outgrowth. This method for immobilizing biomolecules in 3D matrices can generally be applied to any optically clear hydrogel, offering a solution to construct scaffolds with programmed spatial features for tissue engineering applications.

Journal ArticleDOI
TL;DR: This work shows through a comprehensive structural analysis using single-crystal X-ray and powder-synchrotron-radiation diffraction methods, that both the electronic and thermal properties of Zn4Sb3 can be understood in terms of unique structural features that have been previously overlooked.
Abstract: By converting waste heat into electricity, thermoelectric generators could be an important part of the solution to today's energy challenges. The compound Zn_4Sb_3 is one of the most efficient thermoelectric materials known. Its high efficiency results from an extraordinarily low thermal conductivity in conjunction with the electronic structure of a heavily doped semiconductor. Previous structural studies have been unable to explain this unusual combination of properties. Here, we show through a comprehensive structural analysis using single-crystal X-ray and powder-synchrotron-radiation diffraction methods, that both the electronic and thermal properties of Zn_4Sb_3 can be understood in terms of unique structural features that have been previously overlooked. The identification of Sb^(3-) ions and Sb_2^(4-) dimers reveals that Zn_4Sb_3 is a valence semiconductor with the ideal stoichiometry Zn_(13)Sb_(10). In addition, the structure contains significant disorder, with zinc atoms distributed over multiple positions. The discovery of glass-like interstitial sites uncovers a highly effective mechanism for reducing thermal conductivity. Thus Zn_4Sb_3 is in many ways an ideal 'phonon glass, electron crystal' thermoelectric material.

Journal ArticleDOI
TL;DR: It is demonstrated that, in addition to high permittivity, CaCu3Ti4O12 has remarkably strong nonlinear current–voltage characteristics without the addition of any dopants.
Abstract: The discovery of a giant dielectric constant of 10(5) in CaCu(3)Ti(4)O(12) has increased interest in this perovskite-type oxide Here we demonstrate that, in addition to high permittivity, CaCu(3)Ti(4)O(12) has remarkably strong nonlinear current-voltage characteristics without the addition of any dopants An intrinsic electrostatic barrier at the grain boundaries is responsible for the unusual nonlinear behaviour The nonlinear coefficient of CaCu(3)Ti(4)O(12) reaches a value of 900, which is even greater than that of the varistor material ZnO As a result, CaCu(3)Ti(4)O(12) may lead to efficient switching and gas-sensing devices