We characterized the electrical properties of a field-effect transistor (FET) and a nonvolatile memory device based on a solution-processable low bandgap small molecule, Si1TDPP-EE-C6. The small molecule consisted of electron-rich thiophene-dithienosilole-thiophene (Si1T) units and electron-deficient diketopyrrolopyrrole (DPP) units. The as-spun Si1TDPP-EE-C6 FET device exhibited ambipolar transport properties with a hole mobility of 7.3×10(-5) cm2/(Vs) and an electron mobility of 1.6×10(-5) cm2/(Vs). Thermal annealing at 110 °C led to a significant increase in carrier mobility, with hole and electron mobilities of 3.7×10(-3) and 5.1×10(-4) cm2/(Vs), respectively. This improvement is strongly correlated with the increased film crystallinity and reduced π-π intermolecular stacking distance upon thermal annealing, revealed by grazing incidence X-ray diffraction (GIXD) and atomic force microscopy (AFM) measurements. In addition, nonvolatile memory devices based on Si1TDPP-EE-C6 were successfully fabricated by incorporating Au nanoparticles (AuNPs) as charge trapping sites at the interface between the silicon oxide (SiO2) and cross-linked poly(4-vinylphenol) (cPVP) dielectrics. The device exhibited reliable nonvolatile memory characteristics, including a wide memory window of 98 V, a high on/off-current ratio of 1×10(3), and good electrical reliability. Overall, we demonstrate that donor-acceptor-type small molecules are a potentially important class of materials for ambipolar FETs and nonvolatile memory applications.

Bottom-contact bottom-gate organic field-effect transistors (OFETs) are fabricated using a low band gap pDTTDPP-DT polymer as a channel material and single-layer graphene (SLG) or Au source/drain electrodes. The SLG-based ambipolar OFETs significantly outperform the Au-based ambipolar OFETs, and thermal annealing effectively improves the carrier mobilities of the pDTTDPP-DT films. The difference is attributed to the following facts: (i) the thermally annealed pDTTDPP-DT chains on the SLG assume more crystalline features with an edge-on orientation as compared to the polymer chains on the Au, (ii) the morphological features of the thermally annealed pDTTDPP-DT films on the SLG electrodes are closer to the features of those on the gate dielectric layer, and (iii) the SLG electrode provides a flatter, more hydrophobic surface that is favorable for the polymer crystallization than the Au. In addition, the preferred carrier transport in each electrode-based OFET is associated with the HOMO/LUMO alignment relative to the Fermi level of the employed electrode. All of these experimental results consistently explain why the carrier mobilities of the SLG-based OFET are more than 10 times higher than those of the Au-based OTFT. This work demonstrates the strong dependence of ambipolar carrier transport on the source/drain electrode and annealing temperature.

Plasmonic effects that arise from embedding metallic nanoparticles (NPs) in polymer solar cells (PSCs) have been extensively studied. Many researchers have utilized metallic NPs in PSCs by either incorporating them into the PSC interlayers (e.g., the hole extraction and electron extraction layers) or blending them into the bulk heterojunction (BHJ) active layer. In such studies, the dispersity of the metallic NPs in each layer may vary due to both the different nature of the ligands and the amount of ligands on the metallic NPs. This in turn can produce different PSC performance parameters. Here, we systematically control the amount of attached organic ligands on Au NPs to control their dispersion behavior in the BHJ active layer of PSCs. By controlling the number of capping organic ligands on the Au NPs, the dispersity of the NPs in the BHJ layer is also controlled and the positive effects (particularly the plasmonic and electrical effects) of the Au NPs in the PSCs are investigated. From the obtained results, we find that the electrical contribution of the Au NPs is a more dominant factor for enhancing cell efficiency when compared to the plasmonic effect.

A ladder-type poly­(phenyl-co-methacryl silsesquioxane) (PPMSQ) copolymer was developed for use as a gate dielectric in high-performance organic field-effect transistors (OFETs). The ladder-type PPMSQ copolymer was synthesized via the hydrolysis of two types of monomers, methacryloxypropyltrimethoxysilane and phenyltrimethoxysilane, followed by a condensation polymerization. The phenyl groups in one monomer were introduced to enhance the structural ordering of the overlying organic semiconductors, whereas the methacryloxypropyl groups in the other monomer were introduced to cross-link the polymer chains via thermal- or photocuring. The curing process enhanced the electrical strength of the gate dielectric layer due to the formation of a network structure with a reduced free volume. Thermal curing reduced the surface energy of the gate dielectrics, which improved the structural order of the overlying organic semiconductors and promoted the formation of large grains. The ladder-type PPMSQ was used as a gate dielectric to produce benchmark p- and n-channel OFETs based on pentacene and N,N′-dioctyl-3,4,9,10-perylenedicarboximide (PTCDI-C8), respectively. The resulting OFETs exhibited excellent electrical performances, including a high carrier mobility (0.53 cm2 V–1 s–1 for the p-type pentacene OFET and 0.17 cm2 V–1 s–1 for the n-type PTCDI-C8 OFET) and a high ON/OFF current ratio exceeding 104. The photocured patterned PPMSQ film was successfully used to fabricate complementary OFET-based inverters that yielded high gains. The use of the ladder-type PPMSQ gate dielectrics provides a novel approach to realizing next-generation organic electronics.

We synthesized a solution-processable low band gap small molecule, Si1TDPP-EE-COC6, for use as a semiconducting channel material in organic thin film transistors (OTFTs). The Si1TDPP-EE-COC6 is composed of electron-rich thiophene−dithienosilole−thiophene (Si1T) units and electron-deficient diketopyrrolopyrrole (DPP) and carbonyl units. SiTDPP-EE-COC6-based OTFTs with Au source/drain electrodes were fabricated, and their electrical properties were systematically investigated with increasing thermal annealing temperature. The hole and electron mobilities of as-spun Si1TDPP-EE-COC6 were 3.3 × 10 −4 and 1.7 × 10 −4 cm 2 V −1 s −1 , respectively. The carrier mobilities increased significantly upon thermal annealing at 150°C, yielding a hole mobility of 0.003 cm 2 V −1 s −1 and an electron mobility of 0.002 cm 2 V −1 s −1 . The performance enhancement upon thermal annealing was strongly associated with the formation of a layered edge-on structure and a reduction in the π−π intermolecular spacing. Importantly, the use of atomically thin single-layer graphene (SLG) source/drain electrodes that were grown by the chemical vapor deposition (CVD) method further increased the carrier mobilities. The 150°C annealed Si1TDPP-EE-COC6-based OTFTs with SLG source/drain electrodes exhibited a hole mobility of 0.011 cm 2 V −1 s −1 and an electron mobility of 0.015 cm 2 V −1 s −1 . The improved electrical performances of the SLG OTFTs were attributed to the stepless flat surface of the SLG electrodes and the better interfacial contact between the Si1TDPP-EE-COC6 molecules and the SLG electrodes compared to the Au electrodes. This work suggests that careful chemical design is essential to enhance balanced ambipolar transistor performance based on small conjugated molecules, and the SLG is a good electrode material to promote the carrier mobilities.