Electron and ambipolar transport in organic field-effect transistors.

One of the advantages of organic over inorganic semiconductors is they can be grown from solution, but their electrical mobility is often poor. Yuan et al. report a technique for fabricating organic transistors with mobilities far beyond that of amorphous silicon and close to that of polycrystalline silicon.

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Ultra-high mobility transparent organic thin film transistors grown by an off-centre spin-coating method

Principal goals in organic thin-film transistor (OTFT) gate dielectric research include achieving: (i) low gate leakage currents and good chemical/thermal stability, (ii) minimized interface trap state densities to maximize charge transport efficiency, (iii) compatibility with both p- and n- channel organic semiconductors, (iv) enhanced capacitance to lower OTFT operating voltages, and (v) efficient fabrication via solution-phase processing methods. In this Review, we focus on a prominent class of alternative gate dielectric materials: self-assembled monolayers (SAMs) and multilayers (SAMTs) of organic molecules having good insulating properties and large capacitance values, requisite properties for addressing these challenges. We first describe the formation and properties of SAMs on various surfaces (metals and oxides), followed by a discussion of fundamental factors governing charge transport through SAMs. The last section focuses on the roles that SAMs and SAMTs play in OTFTs, such as surface treatments, gate dielectrics, and finally as the semiconductor layer in ultra-thin OTFTs.

Molecular self-assembled monolayers and multilayers for organic and unconventional inorganic thin-film transistor applications

We explore the dependence of the dark current of C60-based organic photovoltaic (OPV) cells on molecular composition and the degree of intermolecular interaction of several molecular donor materials. The saturation dark current density, JS, is an important factor in determining the open circuit voltage, Voc. The Voc values of OPVs show a strong inverse correlation with JS. Donor materials that show evidence for aggregation in their thin-film absorption spectra and polycrystallinity in thin film X-ray diffraction result in a high dark current, and thus a low Voc. In contrast, donor materials with structures that hinder intermolecular π-interaction give amorphous thin films and reduced values of JS, relative to donors with strong intermolecular π-interactions, leading to a high Voc. This work provides guidance for the design of materials and device architectures that maximize OPV cell power conversion efficiency.

Molecular and morphological influences on the open circuit voltages of organic photovoltaic devices.

The performance of semiconducting polymers has been steadily increasing in the last 20 years. Improved control over the microstructure of these materials and a deeper understanding of how the microstructure affects charge transport are partially responsible for such trend. The development and widespread use of techniques that allow to characterize the microstructure of semiconducting polymers is therefore instrumental for the advance of these materials. This article is a review of the characterization techniques that provide information used to enhance the understanding of structure/property relationships in semiconducting polymers. In particular, the applications of optical and X-ray spectroscopy, X-ray diffraction, and scanning probe techniques in this context are described.

Microstructural Characterization and Charge Transport in Thin Films of Conjugated Polymers

We report ambipolar field-effect transistors fabricated from rubrene thin films on SiO2∕Si substrates. The mobilities of both holes and electrons were extremely low, ranging from 2.2×10−6to8.0×10−6cm2∕Vs, due to disorder in the films. Rubrene forms three-dimensional circular islands even at extremely low coverages and x-ray diffraction observations suggest that the film is amorphous. The formation of the conducting channel of the transistor follows the geometric percolation of rubrene islands.

Ambipolar rubrene thin film transistors

The geometrical arrangement of single-molecule-high islands and the contact between them have large roles in determining the electrical properties of field effect transistors (FETs) based on monolayer-scale pentacene thin films. As the pentacene coverage increases through the submonolayer regime there is a percolation transition where islands come into contact and a simultaneous rapid onset of current. At coverages just above the percolation threshold, the electrical properties vary with geometrical changes in the contacts between the pentacene islands. At higher coverages, the FET mobility is much lower than the mobility measured by the van der Pauw method because of high contact resistances in monolayer-scale pentacene film devices. An increase in the van der Pauw mobility of holes as a function of pentacene coverage shows that second layer islands take part in charge transport.

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Channel formation in single-monolayer pentacene thin film transistors

Functional Self-Assembled Monolayers for Optimized Photoinduced Charge Transfer in Organic Field Effect Transistors

Near edge x-ray absorption fine structure (NEXAFS) spectroscopy is used to study the orientation of pentacene molecules within thin films on SiO2 for thicknesses ranging from monolayers to the bulk (150nm). The spectra exhibit a strong polarization dependence of the π* orbitals for all films, which indicates that the pentacene molecules are highly oriented. At all film thicknesses the orientation varies with the rate at which pentacene molecules are deposited, with faster rates favoring a thin film phase with different tilt angles and slower rates leading to a more bulklike orientation. Our NEXAFS results extend previous structural observations to the monolayer regime and to lower deposition rates. The NEXAFS results match crystallographic data if a finite distribution of the molecular orientations is included. Damage to the molecules by hot electrons from soft x-ray irradiation eliminates the splitting between nonequivalent π* orbitals, indicating a breakup of the pentacene molecule.

Orientation of pentacene molecules on SiO2: From a monolayer to the bulk

Silicon nanomembranes (SiNMs) are very thin, large, free-standing or free-floating two-dimensional (2D) single crystals that can variously be flat, rolled into tubes, or made into any number of odd shapes, cut into millions of identical wires, used as conformal sheets, or chopped into tiny pieces. Because SiNMs are mostly surface or interface and little bulk, they have very interesting properties. We describe electrical conductivity in SiNMs. Because of trap states at the Si/SiO2 interface, bulk dopants become irrelevant to electronic transport when the membrane is thin enough. Replacing the oxide at one interface with the clean-Si surface reconstruction dramatically increases the nanomembrane conductivity. We provide a model for this behaviour. The dimer reconstruction surface states provide a means of 'surface doping'. Other materials with proper highest-occupied molecular orbital (HOMO) or lowest-unoccupied molecular orbital (LUMO) bands, when deposited on the Si surface, should produce the same conductivity effect, affording a broad opportunity for membrane-based sensors.

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Byoungnam Park

Papers

Ambipolar rubrene thin film transistors

Channel formation in single-monolayer pentacene thin film transistors

Functional Self-Assembled Monolayers for Optimized Photoinduced Charge Transfer in Organic Field Effect Transistors

Orientation of pentacene molecules on SiO2: From a monolayer to the bulk

Electrical conductivity in silicon nanomembranes