Héctor A. Becerril

Evaluation of Solution-Processed Reduced Graphene Oxide Films as Transparent Conductors

Processable, single-layered graphene oxide (GO) is an intriguing nanomaterial with tremendous potential for electronic applications. We spin-coated GO thin-films on quartz and characterized their sheet resistance and optical transparency using different reduction treatments. A thermal graphitization procedure was most effective, producing films with sheet resistances as low as 10(2) -10(3) Omega/square with 80% transmittance for 550 nm light. Our experiments demonstrate solution-processed GO films have potential as transparent electrodes.

Organic solar cells with solution-processed graphene transparent electrodes

We demonstrate that solution-processed graphene thin films can serve as transparent conductive anodes for organic photovoltaic cells. The graphene electrodes were deposited on quartz substrates by spin coating of an aqueous dispersion of functionalized graphene, followed by a reduction process to reduce the sheet resistance. Small molecular weight organic solar cells can be directly deposited on such graphene anodes. The short-circuit current and fill factor of these devices on graphene are lower than those of control device on indium tin oxide due to the higher sheet resistance of the graphene films. We anticipate that further optimization of the reduction conditions will improve the performance of these graphene anodes.

Organic Light-Emitting Diodes on Solution-Processed Graphene Transparent Electrodes

Theoretical estimates indicate that graphene thin films can be used as transparent electrodes for thin-film devices such as solar cells and organic light-emitting diodes, with an unmatched combination of sheet resistance and transparency. We demonstrate organic light-emitting diodes with solution-processed graphene thin film transparent conductive anodes. The graphene electrodes were deposited on quartz substrates by spin-coating of an aqueous dispersion of functionalized graphene, followed by a vacuum anneal step to reduce the sheet resistance. Small molecular weight organic materials and a metal cathode were directly deposited on the graphene anodes, resulting in devices with a performance comparable to control devices on indium-tin-oxide transparent anodes. The outcoupling efficiency of devices on graphene and indium-tin-oxide is nearly identical, in agreement with model predictions.

Solution coating of large-area organic semiconductor thin films with aligned single-crystalline domains

Solution coating of organic semiconductors offers great potential for achieving low-cost manufacturing of large-area and flexible electronics. However, the rapid coating speed needed for industrial-scale production poses challenges to the control of thin-film morphology. Here, we report an approach--termed fluid-enhanced crystal engineering (FLUENCE)--that allows for a high degree of morphological control of solution-printed thin films. We designed a micropillar-patterned printing blade to induce recirculation in the ink for enhancing crystal growth, and engineered the curvature of the ink meniscus to control crystal nucleation. Using FLUENCE, we demonstrate the fast coating and patterning of millimetre-wide, centimetre-long, highly aligned single-crystalline organic semiconductor thin films. In particular, we fabricated thin films of 6,13-bis(triisopropylsilylethynyl) pentacene having non-equilibrium single-crystalline domains and an unprecedented average and maximum mobilities of 8.1±1.2 cm(2) V(-1) s(-1) and 11 cm(2) V(-1) s(-1). FLUENCE of organic semiconductors with non-equilibrium single-crystalline domains may find use in the fabrication of high-performance, large-area printed electronics.

Polymerase Chain Reaction Based Scaffold Preparation for the Production of Thin, Branched DNA Origami Nanostructures of Arbitrary Sizes

Designs for DNA origami have previously been limited by the size of the available single-stranded genomes for scaffolds. Here we present a straightforward method for the production of scaffold strands having various lengths, using polymerase chain reaction amplification followed by strand separation via streptavidin-coated magnetic beads. We have applied this approach in assembling several distinct DNA nanostructures that have thin ( approximately 10 nm) features and branching points, making them potentially useful templates for nanowires in complex electronic circuitry.

Pentaceno[2,3-b]thiophene, a hexacene analogue for organic thin film transistors.

Hexacene and larger fused rings remain elusive targets for chemists. Here, we report a hexacene-like molecule containing six linearly fused rings, specifically a pentacene molecule fused with a terminal thiophene ring, pentaceno[2,3-b]thiophene. It can be purified and isolated as a purple-black powder at ambient conditions. This molecule has a low HOMO-LUMO gap of 1.75 eV in o-DCB and an optical band gap of 1.58 eV in thin film. Top contact organic thin film transistors (OTFTs) were made, and atomic force microscopy (AFM) reveals a dendritic thin film growth characteristic of pentacene. An OTFT mobility of 0.574 cm(2)/V s was measured for pentaceno[2,3-b]thiophene under nitrogen.

Thiophene-Rich Fused-Aromatic Thienopyrazine Acceptor for Donor-Acceptor Low Band-Gap Polymers for Otft and Polymer Solar Cell Applications

Thiophene enriched fused-aromatic thieno[3,4-b]pyrazine systems were designed and employed to produce low band gap polymers (Eg = 1.0–1.4 eV) when copolymerized with fluorene and cyclopentadithiophene. The copolymers are mainly investigated for organic thin film transistor and organic photovoltaic applications. Molecular packing in the thin films of these polymers was investigated using Grazing incidence X-ray Scattering. Although both fluorene and cyclopentadithiophene polymers follow similar face to face π–π stacking, the latter polymers show much smaller lamellar d-spacings due to side-chain interdigitation between the lamellae. This lead to the higher charge carrier mobilities in cyclopentadithiophene polymers (up to 0.044 cm2/V.s) compared to fluorene polymers (up to 8.1 × 10−3 cm2/V.s). Power conversion efficiency of 1.4% was achieved using fluorene copolymer in solar cells with a fullerene derivative as an acceptor. Although the cyclopentadithiophene polymers show lower band gaps with higher absorption coefficients compared to fluorene copolymers, but the power conversion efficiencies in solar cells of these polymers are low due to their low ionization potentials.

Fabrication and evaluation of solution-processed reduced graphene oxide electrodes for p- and n-channel bottom-contact organic thin-film transistors.

Reduced graphene oxide (RGO) is an electrically conductive carbon-based nanomaterial that has recently attracted attention as a potential electrode for organic electronics. Here we evaluate several solution-based methods for fabricating RGO bottom-contact (BC) electrodes for organic thin-film transistors (OTFTs), demonstrate functional p- and n-channel devices with such electrodes, and compare their electrical performance with analogous devices containing gold electrodes. We show that the morphology of organic semiconductor films deposited on RGO electrodes is similar to that observed in the channel region of the devices and that devices fabricated with RGO electrodes have lower contact resistances compared to those fabricated with gold contacts. Although the conductivity of RGO is poor compared to that of gold, RGO is still an enticing electrode material for organic electronic devices possibly owing to the retention of desirable morphological features, lower contact resistance, lower cost, and solution processability.

Molecular design for improved photovoltaic efficiency: band gap and absorption coefficient engineering

Removing the adjacent thiophene groups around the acceptor core in low band gap polymers significantly enhances solar cell efficiency through increasing the optical absorption and raising the ionization potential of the polymer.

Transistor and solar cell performance of donor–acceptor low bandgap copolymers bearing an acenaphtho[1,2-b]thieno[3,4-e]pyrazine (ACTP) motif

We report the performance of low-bandgap polymers with a new ACTP acceptor in organic transistors (max. field-effect mobility 0.2 cm2V−1s−1), and solar cells (max. efficiency 1.4%).