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A bimodal texturing effect of semiconducting polymers is investigated by incorporating conjugated small molecules to significantly improve the charge transport characteristics via formation of 3D transport pathways. Solution blending of the electron-transporting polymer, poly{[N,N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)} (P(NDI2OD-T2)), with small molecular crystals of tetrathiafulvalene and tetracyanoquinodimethane is used, and the thin film microstructures are studied using a combination of atomic force microscopy, transmission electron microscopy, 2D grazing incidence X-ray diffraction, and surface-sensitive near-edge X-ray absorption fine structure. Blended thin films show edge-on and face-on bimodal texture with long-range order and microstructure packing orientation preferable for electron transport through the channel in organic field-effect transistors, which is confirmed by high electron mobility 1.91 cm2 V−1 s−1, small contact resistance, and low energetic disorder according to temperature dependence of the field-effect mobility. Structural changes suggest a 3D network charge transport model via lamella packing and bimodal orientation of the semiconducting polymers.

A specific design for solution-processed doping of active semiconducting materials would be a powerful strategy in order to improve device performance in flexible and/or printed electronics. Tetrabutylammonium fluoride and tetrabutylammonium hydroxide contain Lewis base anions, F− and OH−, respectively, which are considered as organic dopants for efficient and cost-effective n-doping processes both in n-type organic and nanocarbon-based semiconductors, such as poly[[N,N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)] (P(NDI2OD-T2)) and selectively dispersed semiconducting single-walled carbon nanotubes by π-conjugated polymers. The dramatic enhancement of electron transport properties in field-effect transistors is confirmed by the effective electron transfer from the dopants to the semiconductors as well as controllable onset and threshold voltages, convertible charge-transport polarity, and simultaneously showing excellent device stabilities under ambient air and bias stress conditions. This simple solution-processed chemical doping approach could facilitate the understanding of both intrinsic and extrinsic charge transport characteristics in organic semiconductors and nanocarbon-based materials, and is thus widely applicable for developing high-performance organic and printed electronics and optoelectronics devices.

In this paper, a technique using mixed transition-metal oxides as contact interlayers to modulate both the electron- and hole-injections in ambipolar organic field-effect transistors (OFETs) is presented. The cesium carbonate (Cs2CO3) and vanadium pentoixide (V2O5) are found to greatly and independently improve the charge injection properties for electrons and holes in the ambipolar OFETs using organic semiconductor of diketopyrrolopyrrolethieno[3,2-b]thiophene copolymer (DPPT-TT) and contact electrodes of molybdenum (Mo). When Cs2CO3 and V2O5 are blended at various mixing ratios, they are observed to very finely and constantly regulate the Mo's work function from −4.2 eV to −4.8 eV, leading to high electron- and hole-mobilities as high as 2.6 and 2.98 cm2 V−1 s−1, respectively. The most remarkable finding is that the device characteristics and device performance can be gradually controlled by adjusting the composition of mixed-oxide interlayers, which is highly desired for such applications as complementary circuitry that requires well matched n-channel and p-channel device operations. Therefore, such simple interface engineering in conjunction with utilization of ambipolar semiconductors can truly enable the promising low-cost and soft organic electronics for extensive applications.

The selective tuning of the operational mode from ambipolar to unipolar transport in organic field-effect transistors (OFETs) by printing molecular dopants is reported. The field-effect mobility (μFET) and onset voltage (Von) of both for electrons and holes in initially ambipolar methanofullerene [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) OFETs are precisely modulated by incorporating a small amount of cesium fluoride (CsF) n-type dopant or tetrafluoro-tetracyanoquinodimethane (F4-TCNQ) p-type dopant for n-channel or p-channel OFETs either by blending or inkjet printing of the dopant on the pre-deposited semiconductor. Excess carriers introduced by the chemical doping compensate traps by shifting the Fermi level (EF) toward respective transport energy levels and therefore increase the number of mobile charges electrostatically accumulated in channel at the same gate bias voltage. In particular, n-doped OFETs with CsF show gate-voltage independent Ohmic injection. Interestingly, n- or p-doped OFETs show a lower sensitivity to gate-bias stress and an improved ambient stability with respect to pristine devices. Finally, complementary inverters composed of n- and p-type PCBM OFETs are demonstrated by selective doping of the pre-deposited semiconductor via inkjet printing of the dopants.

The effects of using a blocking dielectric layer and metal nanoparticles (NPs) as charge-trapping sites on the characteristics of organic nano-floating-gate memory (NFGM) devices are investigated. High-performance NFGM devices are fabricated using the n-type polymer semiconductor, poly{[N,N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)} (P(NDI2OD-T2)), and various metal NPs. These NPs are embedded within bilayers of various polymer dielectrics (polystyrene (PS)/poly(4-vinyl phenol) (PVP) and PS/poly(methyl methacrylate) (PMMA)). The P(NDI2OD-T2) organic field-effect transistor (OFET)-based NFGM devices exhibit high electron mobilities (0.4–0.5 cm2 V−1 s−1) and reliable non-volatile memory characteristics, which include a wide memory window (≈52 V), a high on/off-current ratio (Ion/Ioff ≈ 105), and a long extrapolated retention time (>107 s), depending on the choice of the blocking dielectric (PVP or PMMA) and the metal (Au, Ag, Cu, or Al) NPs. The best memory characteristics are achieved in the ones fabricated using PMMA and Au or Ag NPs. The NFGM devices with PMMA and spatially well-distributed Cu NPs show quasi-permanent retention characteristics. An inkjet-printed flexible P(NDI2OD-T2) 256-bit transistor memory array (16 × 16 transistors) with Au-NPs on a polyethylene naphthalate substrate is also fabricated. These memory devices in array exhibit a high Ion/Ioff (≈104 ± 0.85), wide memory window (≈43.5 V ± 8.3 V), and a high degree of reliability.

High-performance top-gated organic fi eld-effect transistor (OFET) memory devices using electrets and their applications to flprinted organic NAND fl ash are reported. The OFETs based on an inkjet-printed p-type polymer semiconductor with effi ciently chargeable dielectric poly(2-vinylnaphthalene) (PVN) and high-k blocking gate dielectric poly(vinylidenefl trifl uoroethylene) (P(VDF-TrFE)) shows excellent non-volatile memory characteristics. The superior memory characteristics originate mainly from reversible charge trapping and detrapping in the PVN electret layer effi ciently in low-k/high-k bilayered dielectrics. A strategy is devised for the successful development of monolithically inkjet-printed fl exible organic NAND fl ash memory through the proper selection of the polymer electrets (PVN or PS), where PVN/- and PS/P(VDF-TrFE) devices are used as non-volatile memory cells and ground- and bit-line select transistors, respectively. Electrical simulations reveal that the fl exible printed organic NAND fl ash can be possible to program, read, and erase all memory cells in the memory array repeatedly without affecting the non-selected memory cells.

Organic field-effect transistor (FET) memory is an emerging technology with the potential to realize light-weight, low-cost, flexible charge storage media. Here, solution-processed poly[9,9-dioctylfluorenyl-2,7-diyl]-co-(bithiophene)] (F8T2) nano floating gate memory (NFGM) with a top-gate/bottom-contact device configuration is reported. A reversible shift in the threshold voltage (V Th ) and reliable memory characteristics was achieved by the incorporation of thin Au nanoparticles (NPs) as charge storage sites for negative charges (electrons) at the interface between polystyrene and cross-linked poly(4-vinylphenol). The F8T2 NFGM showed relatively high field-effect mobility (μ FET ) (0.02 cm 2 V -1 s -1 ) for an amorphous semiconducting polymer with a large memory window (ca. 30 V), a high on/off ratio (more than 10 4 ) during writing and erasing with an operation voltage of 80 V of gate bias in a relatively short timescale (less than 1 s), and a retention time of a few hours. This top-gated polymer NFGM could be used as an organic transistor memory element for organic flash memory.

These func-tionalities arise from field-effect modulation by the chargesstored in chargeable polymer gate dielectrics, referred to aspolymer electrets.An electret is a piece of dielectric material that exhibits aquasi-permanent electrical charges or dipolar polarization,including ferro-, piezo-, and pyro-electric polymers.