RESUMO

In this work, the synthesis of BODIPY-phenyl-triazole labelled coumarins (BPhTCs) using a two-step approach is described. The influence of the BODIPY appending on the photophysical, electrochemical and thermal properties of the phenyl-triazole-coumarin precursors (PhTCs) was investigated. Band gap energies were measured by absorption spectroscopy (2.20 ± 0.02 eV in the solid and 2.35 ± 0.01 eV in solution) and cyclic voltammetry (2.10 ± 0.05 eV). The results are supported by DFT calculations confirming the presence of lowest LUMO levels that facilitate the electron injection and stabilize the electron transport. Their charge-transport parameters were measured in Organic Field-Effect Transistor (OFET) devices. BPhTCs showed an ambipolar transistor behavior with good n-type charge mobilities (10-2 cm2V-1s-1) allowing these derivatives to be employed as promising semiconducting crystalline and fluorescent materials with good thermal and air stability up to 250 °C.

RESUMO

The layer-by-layer (LbL) technique has been proven to be one of the most versatile approaches in order to fabricate functional nanofilms. The use of simple and inexpensive procedures as well as the possibility to incorporate a very wide range of materials through different interactions have driven its application in a wide range of fields. On the other hand, field-effect transistors (FETs) are certainly among the most important elements in electronics. The ability to modulate the flowing current between a source and a drain electrode via the voltage applied to the gate electrode endow these devices to switch or amplify electronic signals, being vital in all of our everyday electronic devices. In this topical review, we highlight different research efforts to engineer field-effect transistors using the LbL assembly approach. We firstly discuss on the engineering of the channel material of transistors via the LbL technique. Next, the deposition of dielectric materials through this approach is reviewed, allowing the development of high-performance electronic components. Finally, the application of the LbL approach to fabricate FETs-based biosensing devices is also discussed, as well as the improvement of the transistor's interfacial sensitivity by the engineering of the semiconductor with polyelectrolyte multilayers.

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In this work, the electronic transport properties of Te roll-like nanostructures were investigated in a broad temperature range by fabricating single-nanostructure back-gated field-effect-transistors via photolithography. These one-dimensional nanostructures, with a unique roll-like morphology, were produced by a facile synthesis and extensively studied by scanning and transmission electron microscopy. The nanostructures are made of pure and crystalline Tellurium with trigonal structure (t-Te), and exhibit p-type conductivity with enhanced field-effect hole mobility between 273 cm2/Vs at 320 K and 881 cm2/Vs at 5 K. The thermal ionization of shallow acceptors, with small ionization energy between 2 and 4 meV, leads to free-hole conduction at high temperatures. The free-hole mobility follows a negative power-law temperature behavior, with an exponent between -1.28 and -1.42, indicating strong phonon scattering in this temperature range. At lower temperatures, the electronic conduction is dominated by nearest-neighbor hopping (NNH) conduction in the acceptor band, with a small activation energy E NNH ≈ 0.6 meV and an acceptor concentration of N A ≈ 1 × 1016 cm-3. These results demonstrate the enhanced electrical properties of these nanostructures, with a small disorder, and superior quality for nanodevice applications.

RESUMO

Organic thin-film transistors (OTFTs) are miniaturized devices based upon the electronic responses of organic semiconductors. In comparison to their conventional inorganic counterparts, organic semiconductors are cheaper, can undergo reversible doping processes and may have electronic properties chiefly modulated by molecular engineering approaches. More recently, OTFTs have been designed as gas sensor devices, displaying remarkable performance for the detection of important target analytes, such as ammonia, nitrogen dioxide, hydrogen sulfide and volatile organic compounds (VOCs). The present manuscript provides a comprehensive review on the working principle of OTFTs for gas sensing, with concise descriptions of devices' architectures and parameter extraction based upon a constant charge carrier mobility model. Then, it moves on with methods of device fabrication and physicochemical descriptions of the main organic semiconductors recently applied to gas sensors (i.e., since 2015 but emphasizing even more recent results). Finally, it describes the achievements of OTFTs in the detection of important gas pollutants alongside an outlook toward the future of this exciting technology.

RESUMO

In the search for gas sensing materials, two-dimensional materials offer the possibility of designing sensors capable of tuning the electronic band structure by controlling their thickness, quantity of dopants, alloying between different materials, vertical stacking, and the presence of gases. Through materials engineering it is feasible to study the electrical properties of two-dimensional materials which are directly related to their crystalline structure, first Brillouin zone, and dispersion energy, the latter estimated through the tight-binding model. A review of the electrical properties directly related to the crystalline structure of these materials is made in this article for the two-dimensional materials used in the design of gas sensors. It was found that most 2D sensing materials have a hexagonal crystalline structure, although some materials have monoclinic, orthorhombic and triclinic structures. Through the simulation of the mathematical models of the dispersion energy, two-dimensional and three-dimensional electronic band structures were predicted for graphene, hexagonal boron nitride (h-BN) and silicene, which must be known before designing a gas sensor.

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We present the construction of layer-by-layer (LbL) assemblies of polyethylenimine and urease onto reduced-graphene-oxide based field-effect transistors (rGO FETs) for the detection of urea. This versatile biosensor platform simultaneously exploits the pH dependency of liquid-gated graphene-based transistors and the change in the local pH produced by the catalyzed hydrolysis of urea. The use of an interdigitated microchannel resulted in transistors displaying low noise, high pH sensitivity (20.3µA/pH) and transconductance values up to 800 µS. The modification of rGO FETs with a weak polyelectrolyte improved the pH response because of its transducing properties by electrostatic gating effects. In the presence of urea, the urease-modified rGO FETs showed a shift in the Dirac point due to the change in the local pH close to the graphene surface. Markedly, these devices operated at very low voltages (less than 500mV) and were able to monitor urea in the range of 1-1000µm, with a limit of detection (LOD) down to 1µm, fast response and good long-term stability. The urea-response of the transistors was enhanced by increasing the number of bilayers due to the increment of the enzyme surface coverage onto the channel. Moreover, quantification of the heavy metal Cu2+(with a LOD down to 10nM) was performed in aqueous solution by taking advantage of the urease specific inhibition.

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RESUMO

Peptide-based nanostructures derived from natural amino acids are superior building blocks for biocompatible devices as they can be used in a bottom-up process without the need for expensive lithography. A dense nanostructured network of l,l-diphenylalanine (FF) was synthesized using the solid-vapor-phase technique. Formation of the nanostructures and structure-phase relationship were investigated by electron microscopy and Raman scattering. Thin films of l,l-diphenylalanine micro/nanostructures (FF-MNSs) were used as the dielectric layer in pentacene-based field-effect transistors (FETs) and metal-insulator-semiconductor diodes both in bottom-gate and in top-gate structures. Bias stress studies show that FF-MNS-based pentacene FETs are more resistant to degradation than pentacene FETs using FF thin film (without any nanostructures) as the dielectric layer when both are subjected to sustained electric fields. Furthermore, it is demonstrated that the FF-MNSs can be functionalized for detection of enzyme-analyte interactions. This work opens up a novel and facile route toward scalable organic electronics using peptide nanostructures as scaffolding and as a platform for biosensing.

Assuntos