Harnessing Intramolecular Chalcogen-Chalcogen Bonding in Merocyanines for Utilization in High-Efficiency Photon-to-Current Conversion Optoelectronics.

A novel series of donor (D)-π-acceptor (A) merocyanine molecules harnessed with intramolecular chalcogen bonding (ChaB) is designed, synthesized, and characterized. ChaB comprises periodic chalcogen atoms, S, Se, and Te, and a neighboring oxygen atom of a carbonyl moiety. Compared to the D-π-A merocyanine dye with nontraditional intramolecular hydrogen bonding, the novel molecules with an intramolecular ChaB exhibit remarkably smaller absorption spectral widths and higher absorption coefficients attributed to their cyanine-like characteristics approaching the resonance parameter (c2) ∼0.5; furthermore, they exhibit better thermal stabilities and electrical charge-carrier transport properties in films. These novel D-π-A merocyanines harnessed with intramolecular ChaB networks are successfully utilized in high-performance color-selective organic photon-to-current conversion optoelectronic devices with excellent thermal stabilities. This study reports that the unique intramolecular ChaB plays an essential role in locking the molecular conformation of merocyanine molecules and enhancing the optical, thermal, and optoelectronic properties of high-performance and high-efficiency organic photon-to-current conversion devices.

Nanotube and poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) composite film for the electrode applications in organic thin-film transistor and dye-sensitized solar cells.

In this study, composite films made of coiled carbon nanotubes (CCNTs) and poly(3,4-ethylenedioxythiophene) polymerized with poly(4-styrenesulfonate) (PEDOT:PSS) were fabricated with different composition ratios. The variations in film properties (including surface morphology, work function, and electrical conductivity) in accordance with the amount of CCNT dosing were investigated. Subsequently, through HCl-methanol treatment, we achieved a significant enhancement in electrical conductivity with little damage to the CCNT features. The characteristics of CCNT/PEDOT:PSS composite film are generally comparable to those of PEDOT:PSS film, and some of them, such as catalytic activity and work function, are significantly higher. On the basis of these versatile features, the CCNT/PEDOT:PSS composite films exhibit excellent performance as source/drain electrode in organic thin-film transistors and as catalytic counter electrode in dye-sensitized solar cells.

Degradation by water vapor of hydrogenated amorphous silicon oxynitride films grown at low temperature.

We report on the degradation process by water vapor of hydrogenated amorphous silicon oxynitride (SiON:H) films deposited by plasma-enhanced chemical vapor deposition at low temperature. The stability of the films was investigated as a function of the oxygen content and deposition temperature. Degradation by defects such as pinholes was not observed with transmission electron microscopy. However, we observed that SiON:H film degrades by reacting with water vapor through only interstitial paths and nano-defects. To monitor the degradation process, the atomic composition, mass density, and fully oxidized thickness were measured by using high-resolution Rutherford backscattering spectroscopy and X-ray reflectometry. The film rapidly degraded above an oxygen composition of ~27 at%, below a deposition temperature of ~150 °C, and below an mass density of ~2.15 g/cm3. This trend can be explained by the extents of porosity and percolation channel based on the ring model of the network structure. In the case of a high oxygen composition or low temperature, the SiON:H film becomes more porous because the film consists of network channels of rings with a low energy barrier.

Polyimide-organosilicate hybrids with improved thermal and optical properties.

Through hydrolysis and polycondensation of amino-silane with alkyl bridged silane, a new type of polysilsesquioxane (PSSQ) was obtained. Here we use amine functionalized silane and bis(silyl)ethane to synthesize alkyl chain linked PSSQ. Compared to conventional polyhedral oligomeric silsesquioxane (POSS), this new silane compound has both enhanced thermal stability and improved compatibility with poly(amic acid). Gelation of this silane compound with poly(amic acid) provides polyimide-organosilicate composite materials. We show that films made from solutions of the composites exhibit higher optical transparency and superior dimensional stability during thermal treatment than films of pure polyimide or of polyimide composites with conventional POSS. Bridging of POSS and chemical bonding between POSS and polyimide chains significantly enhance the physical properties. These results provide useful information for designing molecular architecture for the fabrication of high-performance plastic substrates in the future display devices.