Nanostructured Channel for Improving Emission Efficiency of Hybrid Light-Emitting Field-Effect Transistors.

We report on the mechanism of enhancing the luminance and external quantum efficiency (EQE) by developing nanostructured channels in hybrid (organic/inorganic) light-emitting transistors (HLETs) that combine a solution-processed oxide and a polymer heterostructure. The heterostructure comprised two parts: (i) the zinc tin oxide/zinc oxide (ZTO/ZnO), with and without ZnO nanowires (NWs) grown on the top of the ZTO/ZnO stack, as the charge transport layer and (ii) a polymer Super Yellow (SY, also known as PDY-132) layer as the light-emitting layer. Device characterization shows that using NWs significantly improves luminance and EQE (≈1.1% @ 5000 cd m-2) compared to previously reported similar HLET devices that show EQE < 1%. The size and shape of the NWs were controlled through solution concentration and growth time, which also render NWs to have higher crystallinity. Notably, the size of the NWs was found to provide higher escape efficiency for emitted photons while offering lower contact resistance for charge injection, which resulted in the improved optical performance of HLETs. These results represent a significant step forward in enabling efficient and all-solution-processed HLET technology for lighting and display applications.

Towards Intelligently Designed Evolvable Processors.

Evolution-in-Materio is a computational paradigm in which an algorithm reconfigures a material's properties to achieve a specific computational function. This article addresses the question of how successful and well performing Evolution-in-Materio processors can be designed through the selection of nanomaterials and an evolutionary algorithm for a target application. A physical model of a nanomaterial network is developed which allows for both randomness, and the possibility of Ohmic and non-Ohmic conduction, that are characteristic of such materials. These differing networks are then exploited by differential evolution, which optimises several configuration parameters (e.g., configuration voltages, weights, etc.), to solve different classification problems. We show that ideal nanomaterial choice depends upon problem complexity, with more complex problems being favoured by complex voltage dependence of conductivity and vice versa. Furthermore, we highlight how intrinsic nanomaterial electrical properties can be exploited by differing configuration parameters, clarifying the role and limitations of these techniques. These findings provide guidance for the rational design of nanomaterials and algorithms for future Evolution-in-Materio processors.

Electrical behaviour and evolutionary computation in thin films of bovine brain microtubules.

We report on the electrical behaviour of thin films of bovine brain microtubules (MTs). For samples in both their dried and hydrated states, the measured currents reveal a power law dependence on the applied DC voltage. We attribute this to the injection of space-charge from the metallic electrode(s). The MTs are thought to form a complex electrical network, which can be manipulated with an applied voltage. This feature has been exploited to undertake some experiments on the use of the MT mesh as a medium for computation. We show that it is possible to evolve MT films into binary classifiers following an evolution in materio approach. The accuracy of the system is, on average, similar to that of early carbon nanotube classifiers developed using the same methodology.

Optical properties and carrier dynamics in Co-doped ZnO nanorods.

The controlled modification of the electronic properties of ZnO nanorods via transition metal doping is reported. A series of ZnO nanorods were synthesized by chemical bath growth with varying Co content from 0 to 20 atomic% in the growth solution. Optoelectronic behavior was probed using cathodoluminescence, time-resolved luminescence, transient absorbance spectroscopy, and the incident photon-to-current conversion efficiency (IPCE). Analysis indicates the crucial role of surface defects in determining the electronic behavior. Significantly, Co-doping extends the light absorption of the nanorods into the visible region, increases the surface defects, and shortens the non-radiative lifetimes, while leaving the radiative lifetime constant. Furthermore, for 1 atomic% Co-doping the IPCE of the ZnO nanorods is enhanced. These results demonstrate that doping can controllably tune the functional electronic properties of ZnO nanorods for applications.

Cobalt-Doped ZnO Nanorods Coated with Nanoscale Metal-Organic Framework Shells for Water-Splitting Photoanodes.

Developing highly efficient and stable photoelectrochemical (PEC) water-splitting electrodes via inexpensive, liquid phase processing is one of the key challenges for the conversion of solar energy into hydrogen for sustainable energy production. ZnO represents one the most suitable semiconductor metal oxide alternatives because of its high electron mobility, abundance, and low cost, although its performance is limited by its lack of absorption in the visible spectrum and reduced charge separation and charge transfer efficiency. Here, we present a solution-processed water-splitting photoanode based on Co-doped ZnO nanorods (NRs) coated with a transparent functionalizing metal-organic framework (MOF). The light absorption of the ZnO NRs is engineered toward the visible region by Co-doping, while the MOF significantly improves the stability and charge separation and transfer properties of the NRs. This synergetic combination of doping and nanoscale surface functionalization boosts the current density and functional lifetime of the photoanodes while achieving an unprecedented incident photon to current efficiency (IPCE) of 75% at 350 nm, which is over 2 times that of pristine ZnO. A theoretical model and band structure for the core-shell nanostructure is provided, highlighting how this nanomaterial combination provides an attractive pathway for the design of robust and highly efficient semiconductor-based photoanodes that can be translated to other semiconducting oxide systems.

Controlling the growth of single crystal ZnO nanowires by tuning the atomic layer deposition parameters of the ZnO seed layer.

Semiconducting nanowires (NWs) offer exciting prospects for a wide range of technological applications. The translation of NW science into technology requires reliable high quality large volume production. This study provides an in-depth investigation of the parameters using an atomic layer deposition system to grow zinc oxide (ZnO) seed layers followed by the chemical bath deposition (CBD) of ZnO NWs to demonstrate the low-cost production of uniform single crystal wurtzite phase ZnO NWs that is scalable to large area substrates. The seed layer texture and the morphology of the NWs grown were systematically investigated using atomic force microscopy as a function of the seed layer deposition parameters. It is shown that the NWs growth orientation can be controlled by tuning the seed layer deposition parameters while maintaining the same CBD conditions. Likewise, the diameters and the surface densities of the NWs varied from 23 to 56 nm and 40 to 327 NWs µm-2, respectively. Significantly, the relationship between the seed layer structure and the NW density indicates a clear correlation between the density of seed layer surface features and the resulting surface NW density of NWs grown.

Model for large-area monolayer coverage of polystyrene nanospheres by spin coating.

Nanosphere lithography, an inexpensive and high throughput technique capable of producing nanostructure (below 100 nm feature size) arrays, relies on the formation of a monolayer of self-assembled nanospheres, followed by custom-etching to produce nanometre size features on large-area substrates. A theoretical model underpinning the self-ordering process by centrifugation is proposed to describe the interplay between the spin speed and solution concentration. The model describes the deposition of a dense and uniform monolayer by the implicit contribution of gravity, centrifugal force and surface tension, which can be accounted for using only the spin speed and the solid/liquid volume ratio. We demonstrate that the spin recipe for the monolayer formation can be represented as a pathway on a 2D phase plane. The model accounts for the ratio of polystyrene nanospheres (300 nm), water, methanol and surfactant in the solution, crucial for large area uniform and periodic monolayer deposition. The monolayer is exploited to create arrays of nanoscale features using 'short' or 'extended' reactive ion etching to produce 30-60 nm (diameter) nanodots or 100-200 nm (diameter) nanoholes over the entire substrate, respectively. The nanostructures were subsequently utilized to create master stamps for nanoimprint lithography.

Direct growth of Si nanowires on flexible organic substrates.

A key characteristic of semiconductor nanowires (NWs) is that they grow on any substrate that can withstand the growth conditions, paving the way for their use in flexible electronics. We report on the direct growth of crystalline silicon nanowires on polyimide substrates. The Si NWs are grown by plasma-enhanced chemical vapor deposition, which allows the growth to proceed at temperatures low enough to be compatible with plastic substrates (350 °C), where gold or indium are used as growth seeds. In is particularly interesting as the seed not only because it leads to a better NW crystal quality but also because it overcomes a core problem induced by the use of Au in silicon processing, i.e. Au creates deep carrier traps when incorporated in the nanowires.

Scanning thermal microscopy with heat conductive nanowire probes.

Scanning thermal microscopy (SThM), which enables measurement of thermal transport and temperature distribution in devices and materials with nanoscale resolution is rapidly becoming a key approach in resolving heat dissipation problems in modern processors and assisting development of new thermoelectric materials. In SThM, the self-heating thermal sensor contacts the sample allowing studying of the temperature distribution and heat transport in nanoscaled materials and devices. The main factors that limit the resolution and sensitivities of SThM measurements are the low efficiency of thermal coupling and the lateral dimensions of the probed area of the surface studied. The thermal conductivity of the sample plays a key role in the sensitivity of SThM measurements. During the SThM measurements of the areas with higher thermal conductivity the heat flux via SThM probe is increased compared to the areas with lower thermal conductivity. For optimal SThM measurements of interfaces between low and high thermal conductivity materials, well defined nanoscale probes with high thermal conductivity at the probe apex are required to achieve a higher quality of the probe-sample thermal contact while preserving the lateral resolution of the system. In this paper, we consider a SThM approach that can help address these complex problems by using high thermal conductivity nanowires (NW) attached to a tip apex. We propose analytical models of such NW-SThM probes and analyse the influence of the contact resistance between the SThM probe and the sample studied. The latter becomes particularly important when both tip and sample surface have high thermal conductivities. These models were complemented by finite element analysis simulations and experimental tests using prototype probe where a multiwall carbon nanotube (MWCNT) is exploited as an excellent example of a high thermal conductivity NW. These results elucidate critical relationships between the performance of the SThM probe on one hand and thermal conductivity, geometry of the probe and its components on the other. As such, they provide a pathway for optimizing current SThM for nanothermal studies of high thermal conductivity materials. Comparison between experimental and modeling results allows us to provide direct estimates of the contact thermal resistances for various interfaces such as MWCNT-Al (5×10(-9)±1×10(-9)Km(2)W(-1)), Si3N4-Al (6×10(-8)±2.5×10(-8)Km(2)W(-1)) and Si3N4-graphene (~10(-8)Km(2)W(-1)). It was also demonstrated that the contact between the MWCNT probe and Al is relatively perfect, with a minimal contact resistance. In contrast, the thermal resistance between a standard Si3N4 SThM probe and Al is an order of magnitude higher than reported in the literature, suggesting that the contact between these materials may have a multi-asperity nature that can significantly degrade the contact resistance.

Nanoscale resolution scanning thermal microscopy using carbon nanotube tipped thermal probes.

We present an experimental proof of concept of scanning thermal nanoprobes that utilize the extreme thermal conductance of carbon nanotubes (CNTs) to channel heat between the probe and the sample. The integration of CNTs into scanning thermal microscopy (SThM) overcomes the main drawbacks of standard SThM probes, where the low thermal conductance of the apex SThM probe is the main limiting factor. The integration of CNTs (CNT-SThM) extends SThM sensitivity to thermal transport measurement in higher thermal conductivity materials such as metals, semiconductors and ceramics, while also improving the spatial resolution. Investigation of thermal transport in ultra large scale integration (ULSI) interconnects, using the CNT-SThM probe, showed fine details of heat transport in ceramic layers, vital for mitigating electromigration in ULSI metallic current leads. For a few layer graphene, the heat transport sensitivity and spatial resolution of the CNT-SThM probe demonstrated significantly superior thermal resolution compared to that of standard SThM probes achieving 20-30 nm topography and ~30 nm thermal spatial resolution compared to 50-100 nm for standard SThM probes. The outstanding axial thermal conductivity, a high aspect ratio and robustness of CNTs can make CNT-SThM the perfect thermal probe for the measurement of nanoscale thermophysical properties and an excellent candidate for the next generation of thermal microscopes.

Electrical behavior of Langmuir-Blodgett networks of sorted metallic and semiconducting single-walled carbon nanotubes.

Langmuir-Blodgett deposition has been used to form thin film networks of both metallic and semiconducting single-walled carbon nanotubes. These have been investigated to understand their physical, optical, and morphological properties. The electrical conductivities over the temperature range 80-350 K and across electrode gaps of 220 nm and 2 mm have been explored. In the case of semiconducting tubes, the results suggest that Poole-Frenkel conduction is the dominant electrical process at temperatures below 150 K and electric fields of greater than 1 MV m(-1). Metallic nanotube networks exhibit a decrease in resistance with a reduction in temperature. This can be approximated by a linear relationship, giving a temperature coefficient of resistance of 10(-3) K(-1).

Direct nanoscale imaging of ballistic and diffusive thermal transport in graphene nanostructures.

We report direct imaging of nanoscale thermal transport in single and few-layer graphene with approximately 50 nm lateral resolution using high vacuum scanning thermal microscopy. We observed increased heat transport in suspended graphene where heat is conducted by ballistic phonons, compared to adjacent areas of supported graphene, and observed decreasing thermal conductance of supported graphene with increased layer number. Our nanothermal images suggest a mean-free-path of thermal phonons in supported graphene below 100 nm.