Organic semiconductors have been the subject of active research for over a decade now, with applications emerging in light-emitting displays and printable electronic circuits. One characteristic feature of these materials is the strong trapping of electrons but not holes: organic field-effect transistors (FETs) typically show p-type, but not n-type, conduction even with the appropriate low-work-function electrodes, except for a few special high-electron-affinity or low-bandgap organic semiconductors. Here we demonstrate that the use of an appropriate hydroxyl-free gate dielectric--such as a divinyltetramethylsiloxane-bis(benzocyclobutene) derivative (BCB; ref. 6)--can yield n-channel FET conduction in most conjugated polymers. The FET electron mobilities thus obtained reveal that electrons are considerably more mobile in these materials than previously thought. Electron mobilities of the order of 10(-3) to 10(-2) cm(2) V(-1) s(-1) have been measured in a number of polyfluorene copolymers and in a dialkyl-substituted poly(p-phenylenevinylene), all in the unaligned state. We further show that the reason why n-type behaviour has previously been so elusive is the trapping of electrons at the semiconductor-dielectric interface by hydroxyl groups, present in the form of silanols in the case of the commonly used SiO2 dielectric. These findings should therefore open up new opportunities for organic complementary metal-oxide semiconductor (CMOS) circuits, in which both p-type and n-type behaviours are harnessed.

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We introduce a method to fabricate high-performance field-effect transistors on the surface of freestanding organic single crystals. The transistors are constructed by laminating a monolithic elastomeric transistor stamp against the surface of a crystal. This method, which eliminates exposure of the fragile organic surface to the hazards of conventional processing, enables fabrication of rubrene transistors with charge carrier mobilities as high as approximately 15 cm2/V.s and subthreshold slopes as low as 2nF.V/decade.cm2. Multiple relamination of the transistor stamp against the same crystal does not affect the transistor characteristics; we exploit this reversibility to reveal anisotropic charge transport at the basal plane of rubrene.

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Spin-coated poly(9,9-di-n-octylfluorene-alt-benzothiadiazole) (F8BT) films of different molecular weights (Mn= 9-255 kg/mol), both in the pristine and annealed state, were studied in an effort to elucidate changes in the polymer packing structure and the effects this structure has on the optoelectronic and charge transport properties of these films. A model based on quantum chemical calculations, wide-angle X-ray scattering, atomic force microscopy, Raman spectroscopy, photoluminescence, and electron mobility measurements was developed to describe the restructuring of the polymer film as a function of polymer chain length and annealing. In pristine high molecular weight films, the polymer chains exhibit a significant torsion angle between the F8 and BT units, and the BT units in neighboring chains are close to one another. Annealing films to sufficiently high transition temperatures allows the polymers to adopt a lower energy configuration in which the BT units in one polymer chain are adjacent to F8 units in a neighboring chain ("alternating structure"), and the torsion angle between F8 and BT units is reduced. This restructuring, dictated by the strong dipole on the BT unit, subsequently affects the efficiencies of interchain electron transfer and exciton migration. Films exhibiting the alternating structure show significantly lower electron mobilities than those of the pristine high molecular weight films, due to a decrease in the efficiency of interchain electron transport in this structure. In addition, interchain exciton migration to low energy weakly emissive states is also reduced for these alternating structure films, as observed in their photoluminescence spectra and efficiencies.

We developed different strategies toward the synthesis of colloidal nanocrystals stabilized with molecular metal chalcogenide complexes (MCCs). Negatively charged MCCs, such as SnS(4)(4-), Sn(2)S(6)(4-), SnTe(4)(4-), AsS(3)(3-), MoS(4)(2-), can quantitatively replace the organic ligands at the nanocrystal surface and stabilize nanocrystal solutions in different polar media. We showed that all-inorganic nanocrystals composed of metals, semiconductors, or magnetic materials and capped with various MCC ligands can be synthesized using convenient and inexpensive chemicals and environmentally benign solvents such as water, formamide, or dimethylsulfoxide. The development of mild synthetic routes was found to be crucial for the design of highly luminescent all-inorganic nanocrystals, such as CdSe/ZnS and PbS capped with Sn(2)S(6)(4-) MCCs, respectively. We also prepared conductive and luminescent layer-by-layer assemblies from inorganically capped colloidal nanocrystals and polyelectrolytes. In close-packed films of 5-nm Au nanocrystals stabilized with Na(2)Sn(2)S(6) we observed very high electrical conductivities (>1000 S cm(-1)).

Bright, ambipolar, light‐emitting polymer field‐effect transistors in a bottom‐contact/top‐gate structure using poly(9,9‐di‐n‐octylfluorene‐alt‐ benzothiadiazole) (F8BT) as a green‐emitting semiconductor show balanced hole and electron mobilities, depending on the polymer dielectric. The emission zone, observed as a bright line in the figure, is well defined and can be moved through the channel.

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