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Methacrylate monomers functionalized with pendant carbazole and oxadiazole moieties were copolymerized into random copolymers with varying carbazole/oxadiazole ratios. Specifically, the monomers of 2-(9H-carbazol-9-yl)ethyl 2-methylacrylate (CE) and 4-[5-(4-tert-butylphenyl)-1,3,4-oxadiazol-2-yl]phenyl 2-methylacrylate (tBPOP) were copolymerized in various ratios, and the inherent hole drift mobilities were assessed through time-of-flight techniques. At a field strength of 345 kV/cm, the homopolymer PCE exhibited a hole mobility of 5.9 x 10(-7) cm(2)/V.s, which was approximately twice the value of the technologically important poly(9-vinylcarbazole), which exhibited a value of 2.8 x 10(-7) cm(2)/V.s. The range of hole mobilities in the copolymers varied from 2.4 x 10(-8) cm(2)/V.s for copolymers containing 50 mol % of the carbazole-containing monomer residue to 3.0 x 10(-7) cm(2)/V.s for copolymers that incorporated 88 mol % of the residue. Density functional theory (B3LYP/6-21G*) and optical absorption derived highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energies of CE were -5.39 and -1.94 eV, respectively, while the corresponding oxadiazole monomer (tBPOP) had a HOMO energy of -5.99 eV and a LUMO energy of -2.23 eV. The mean luminous efficiency of coumarin 6 doped single-layer devices constructed from the poly(CE-co-tBPOP) copolymers indicated a relatively flat efficiency of ca. 0.25 cd/A over a wide carbazole mole fraction content of 0.30-0.70.
ACS Appl Mater Interfaces 2009 Apr
PMID:Copolymers of 2-(9H-carbazol-9-yl)ethyl 2-methylacrylate and 4-[5-(4-tert-butylphenyl)-1,3,4-oxadiazol-2-yl]phenyl 2-methylacrylate: correlating hole drift mobility and electronic structure calculations with electroluminescence. 2035 14

The charge-carrier transport in the structures formed at the surface of various conjugated polymer films is investigated by constructing organic thin-film transistors using a novel and simple contact film transfer method. Thin-film transistors prepared by this transfer process have higher field-effect mobility values compared with conventional spin-coated devices for all the studied polymers. In contrast to previous reports, the hole mobility in regioregular poly(3-alkylthiophene)s does not depend on the length of the alkyl chain when the contact film transfer method is used. These results suggest that the thiophene rings adopt a highly ordered edge-on orientation and strong interchain pi-pi interactions spontaneously form at the polymer/air interface during the spin coating.
ACS Appl Mater Interfaces 2009 Nov
PMID:Enhanced charge transport in polymer thin-film transistors prepared by contact film transfer method. 2035 40

Nanocomposite matrices of silver/poly(3-hexylthiophene) (P3HT) were prepared in ultrahigh vacuum through vapor-phase codeposition. Change in microstructure, chemical nature, and electronic properties with increasing filler (Ag) content were investigated using in situ XPS and UPS, and ambient AFM. At least two chemical binding states occur between Ag nanoparticles and sulfur in P3HT at the immediate contact layer, but no evidence of interaction between Ag and carbon (in P3HT) was found. AFM images reveal a change in Ag nanoparticles size with concentration which modifies the microstructure and the average roughness of the surface. Under codeposition, P3HT largely retains its conjugated structures, which is evidenced by the similar XPS and UPS spectra to those of P3HT films deposited on other substrates. We demonstrate here that the magnitude of the barrier height for hole injection (epsilon(v)(F)) and the position of the highest occupied band edge (HOB) with respect to the Fermi level of Ag may be controlled and changed by adjusting the metal (Ag) content in the composite. Furthermore, UPS reveals distinct features related to the C 2p (sigma states) in the 5-12 eV regions, indicating the presence of ordered P3HT, which is different from solution processed films.
ACS Appl Mater Interfaces 2009 Dec
PMID:Photoemission spectroscopy and atomic force microscopy investigation of vapor-phase codeposited silver/poly(3-hexylthiophene) composites. 2035 49

Hierarchically structured titania films for application in hybrid solar cells are prepared by combining microsphere templating and sol-gel chemistry with an amphiphilic diblock copolymer as a structure-directing agent. The films have a functional structure on three size scales: (1) on the micrometer scale a holelike structure for reduction of light reflection, (2) on an intermediate scale macropores for surface roughening and improved infiltration of a hole transport material, and (3) on a nanometer scale a mesoporous structure for charge generation. Poly(dimethyl siloxane)-block-methyl methacrylate poly(ethylene oxide) (PDMS-b-MA(PEO)) is used as a structure-directing agent for the preparation of the mesopore structure, and poly(methyl methacrylate) (PMMA) microspheres act as a template for the micrometer-scale structure. The structure on all levels is modified by the method of polymer extraction as well as by the addition of PMMA particles to the sol-gel solution. Calcination results in structures with increased size and a higher degree of order than extraction with acetic acid. With addition of PMMA a microstructure is created and the size of the mesopores is reduced. Already moderate microstructuring results in a strong decrease in film reflectivity; a minimum reflectivity value of less than 0.1 is obtained by acetic acid treatment and subsequent calcination.
ACS Appl Mater Interfaces 2009 Dec
PMID:Hierarchically structured titania films prepared by polymer/colloidal templating. 2035 68

The dependence of pentacene nanostructures on gate dielectric surfaces were investigated for flexible organic field-effect transistor (OFET) applications. Two bilayer types of polymer/aluminum oxide (Al(2)O(3)) gate dielectrics were fabricated on commercial Al foils laminated onto a polymer back plate. Some Al foils were directly used as gate electrodes, and others were smoothly polished by an electrolytic etching. These Al surfaces were then anodized and coated with poly(alpha-methyl styrene) (PAMS). For PAMS/Al(2)O(3) dielectrics onto etched Al foils, surface roughness up to approximately 1 nm could be reached, although isolated dimples with a lateral diameter of several micrometers were still present. On PAMS/Al(2)O(3) dielectrics (surface roughness >40 nm) containing mechanical grooves of Al foil, average hole mobility (mu(FET)) of 50 nm thick pentacene-FETs under the low operating voltages (|V| < 6 V) was approximately 0.15 cm(2) V(-1) s(-1). In contrast, pentacene-FETs employing the etched Al gates exhibited mu(FET) of approximately 0.39 cm(2) V(-1) s(-1), which was comparable to that of reference samples with PAMS/Al(2)O(3) dielectrics onto flat sputtered Al gates. Conducting-probe atomic force microscopy and two-dimensional X-ray diffraction of pentacene films with various thicknesses revealed different out-of-plane and in-plane crystal orderings of pentacene, depending on the surface roughness of the gate dielectrics.
ACS Appl Mater Interfaces 2010 Feb
PMID:Dependence of pentacene crystal growth on dielectric roughness for fabrication of flexible field-effect transistors. 2035 84

The morphology of the photoactive layer used in the bulk heterojunction photovoltaic devices is crucial for efficient charge generation and their collection at the electrodes. We investigated the solvent vapor annealing and thermal annealing effect of an alternating phenylenevinylene copolymer P:PCBM blend on its morphology and optical properties. The UV-visible absorption spectroscopy shows that both solvent and thermal annealing can result in self-assembling of copolymer P to form an ordered structure, leading to enhanced absorption in the red region and hole transport enhancement. By combining the solvent and thermal annealing of the devices, the power conversion efficiency is improved. This feature was attributed to the fact that the PCBM molecules begin to diffuse into aggregates and together with the ordered copolymer P phase form bicontinuous pathways in the entire layer for efficient charge separation and transport. Furthermore, the measured photocurrent also suggests that the space charges no longer limit the values of the short circuit current (J(sc)) and fill factor (FF) for solvent-treated and thermally annealed devices. These results indicate that the higher J(sc) and PCE for the solvent-treated and thermally annealed devices can be attributed to the phase separation of active layers, which leads to a balanced carrier mobility. The overall PCE of the device based on the combination of solvent annealing and thermal annealing is about 3.7 %.
ACS Appl Mater Interfaces 2010 Feb
PMID:Effect of solvent and subsequent thermal annealing on the performance of phenylenevinylene copolymer: PCBM solar cells. 2035 98

The donor, 2,4-bis[4-(N,N-diisobutylamino)-2,6-dihydroxyphenyl] squaraine (SQ) is used with the acceptor, [6,6]-phenyl C70 butyric acid methyl ester (PC70BM) to result in efficient, solution-processed, small-molecule bulk heterojunction photovoltaic cells. The distribution of the donor nanoparticles in the acceptor matrix as a function of relative concentrations results in a trade-off between exciton dissociation and hole mobility (and hence, cell series resistance). A bulk heterojunction solar cell consisting of an active region with a component ratio of SQ to PC70BM of 1:6 has a power conversion efficiency of 2.7 +/- 0.1% with a 8.85 +/- 0.22 mA/cm(2) short-circuit current density and an open-circuit voltage of 0.89 +/- 0.01 V obtained under simulated 1 sun (100 mW/cm(2)) air mass 1.5 global (AM1.5 G) solar illumination. This is a decrease from 3.3 +/- 0.3% at 0.2 sun intensity, and is less than that of a control planar heterojunction SQ/C60 cell with 4.1 +/- 0.2% at 1 sun, suggesting that the nanoparticle morphology introduces internal resistance into the solution-based thin film. The nanomorphology and hole mobility in the films is strongly dependent on the SQ-to-PC70BM ratio, increasing by greater than 2 orders of magnitude as the ratio increases from 28% to 100% SQ.
ACS Nano 2010 Apr 27
PMID:Solution-processed squaraine bulk heterojunction photovoltaic cells. 2035 89

We show that ligand exchange with short-chain carboxylic acids (formic, acetic, and oxalic acid) can quantitatively remove oleic acid from the surface of PbSe and PbS quantum dot (QD) films to yield p-type, carboxylate-capped QD solids with field-effect hole mobilities in the range of 10(-4)-10(-1) cm(2) V(-1) s(-1). For a given chemical treatment, PbSe devices have 10-fold higher mobilities than PbS devices because of stronger electronic coupling among the PbSe QDs and possibly a lower density of surface traps. Long-term optical and electrical measurements (i) show that carboxylate-capped PbSe QD films oxidize much more gradually in air than do thiol-capped PbSe films and (ii) quantify the slower and less extensive oxidation of PbS relative to PbSe QDs. We find that whereas the hole mobility of thiol-capped samples decreases continuously with time in air, the mobility of carboxylate-capped films first increases by an order of magnitude over several days before slowly decreasing over weeks. This behavior is a consequence of the more robust binding of carboxylate ligands to the QD surface, such that adsorbed oxygen and water initially boost the hole mobility by passivating surface states and only slowly degrade the ligand passivation to establish an oxide shell around each QD in the film. The superior hole mobilities and oxidation resistance of formic- and acetic-treated QD solids may prove useful in constructing efficient, stable QD photovoltaic devices.
ACS Nano 2010 Apr 27
PMID:p-Type PbSe and PbS quantum dot solids prepared with short-chain acids and diacids. 2035 35

The charge mobility in a new hole transporting polymer, poly(2,6-bis(thiophene-2-yl)-3,5-dipentadecyldithieno[3,2-b;2',3'-d]thiophene) (PBTDTT-15), and its blend with (6,6)-phenyl-C(70)-butyric acid methyl ester (PC(70)BM) in a weight ratio of 1:3 at ambient atmosphere condition was investigated using time-of-flight (TOF) photoconductivity and photoinduced charge extraction by linearly increasing voltage (PhotoCELIV) techniques. The bulk heterojunction based photovoltaic (PV) blend (PBTDTT-15:PC(70)BM (1:3)) exhibited a promising power conversion efficiency (PCE) of 3.23% under air mass 1.5 global (AM 1.5G) illumination of 100mW/cm(2). The charge mobility and recombination properties of the best performing cells were investigated. The hole mobility in the pure PBTDTT-15 was in the range of 4 x 10(-4) cm(2)/(V s), which was reduced almost 5 times in the PBTDTT-15:PC(70)BM (1:3) blend. The PhotoCELIV transient observed for the photovoltaic (PV) blend was dominated by electrons, with the charge mobility of the order of 10(-3) cm(2)/(V s), and a weak shoulder at a long time scale due to holes. The effective bimolecular recombination coefficient (beta) obtained for the PV blend deviated significantly from the Langevin recombination coefficient (beta(L)) indicating a phase-separated morphology. The obtained results indicate that the PBTDTT-15:PC(70)BM blend can be potential for organic solar cell applications.
ACS Appl Mater Interfaces 2010 May
PMID:Charge mobility and recombination in a new hole transporting polymer and its photovoltaic blend. 2041 40

A simple, cost-effective, two-step method was proposed for preparing single-phase SnO polycrystalline thin films on quartz. X-ray diffraction (XRD) analysis demonstrated that the annealed films were consisted of polycrystalline alpha-SnO phase without preferred orientation, and chemical composition analysis of the single phase in nature was analyzed using X-ray photoelectron spectroscopy (XPS). Transmittance spectra in UV-vis-IR range indicated that the average transmittance of both the as-deposited and the annealed SnO thin films was up to 70%. The optical band gap decreased from 3.20 to 2.77 eV after the annealing process, which was attributed to the crystalline size related quantum size effect. Photoluminescence (PL) spectrum of the annealed film showed only a weak peak at 585 nm, and no intrinsic optical transition emission was observed. Moreover, the p-type conductivity of SnO film was confirmed through Hall effect measurement, with Hall mobility of 1.4 cm(2) V(-1) s(-1) and hole concentration of 2.8 x 10(16) cm(-3).
ACS Appl Mater Interfaces 2010 Apr
PMID:Microstructural, optical, and electrical properties of SnO thin films prepared on quartz via a two-step method. 2042 26


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