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2.
Angew Chem Int Ed Engl ; 53(47): 12870-5, 2014 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-25264304

RESUMO

Cost-effective, solution-processable organic photovoltaics (OPV) present an interesting alternative to inorganic silicon-based solar cells. However, one of the major remaining challenges of OPV devices is their lack of long-term operational stability, especially at elevated temperatures. The synthesis of a fullerene dumbbell and its use as an additive in the active layer of a PCDTBT:PCBM-based OPV device is reported. The addition of only 20 % of this novel fullerene not only leads to improved device efficiencies, but more importantly also to a dramatic increase in morphological stability under simulated operating conditions. Dynamic secondary ion mass spectrometry (DSIMS) and TEM are used, amongst other techniques, to elucidate the origins of the improved morphological stability.

3.
J Phys Chem A ; 118(45): 10380-90, 2014 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-25154428

RESUMO

The photo- and electroluminescent properties of single-layer two-component blends composed of one blue emitter polymer and one green emitter polymer were studied. The blue emitter, poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-co-(9,9-di-{5'-pentanyl}-fluorenyl-2,7-diyl)] (PFOFPen), was used as the matrix, and the green emitter, poly[(9,9-dihexylfluorenyl-2,7-diyl)-alt-co-(bithiophene)] (F6T2), was used as the guest. The F6T2 content in the blends varied from 0.0075 wt % to 2.4 wt %. Remarkable differences were observed between the electroluminescent (EL) and photoluminescent (PL) spectra of these blends, which indicated that the mechanism for excited-state generation in the former process had a higher efficiency in the aggregated phase than in the nonaggregated phase. Blending these two polymers gradually tuned the emission color from blue (PFOFPen and blends with <0.75 wt % F6T2) to green (F6T2 and blends with >0.75 wt % F6T2). The photophysical processes involved in both EL and PL emission are also discussed.

4.
J Am Chem Soc ; 136(33): 11578-81, 2014 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-25056482

RESUMO

A new tetracyclic lactam building block for polymer semiconductors is reported that was designed to combine the many favorable properties that larger fused and/or amide-containing building blocks can induce, including improved solid-state packing, high charge carrier mobility, and improved charge separation. Copolymerization with thiophene resulted in a semicrystalline conjugated polymer, PTNT, with a broad bandgap of 2.2 eV. Grazing incidence wide-angle X-ray scattering of PTNT thin films revealed a strong tendency for face-on π-stacking of the polymer backbone, which was retained in PTNT:fullerene blends. Corresponding solar cells featured a high open-circuit voltage of 0.9 V, a fill factor around 0.6, and a power conversion efficiency as high as 5% for >200 nm thick active layers, regardless of variations in blend stoichiometry and nanostructure. Moreover, efficiencies of >4% could be retained when thick active layers of ∼400 nm were employed. Overall, these values are the highest reported for a conjugated polymer with such a broad bandgap and are unprecedented in materials for tandem and particularly ternary blend photovoltaics. Hence, the newly developed tetracyclic lactam unit has significant potential as a conjugated building block in future organic electronic materials.

5.
J Phys Chem A ; 116(17): 4285-95, 2012 May 03.
Artigo em Inglês | MEDLINE | ID: mdl-22471613

RESUMO

Fluorene-based systems have shown great potential as components in organic electronics and optoelectronics (organic photovoltaics, OPVs, organic light emitting diodes, OLEDs, and organic transistors, OTFTs). These systems have drawn attention primarily because they exhibit strong blue emission associated with relatively good thermal stability. It is well-known that the electronic properties of polymers are directly related to the molecular conformations and chain packing of polymers. Here, we used three oligofluorenes (trimer, pentamer, and heptamer) as model systems to theoretically investigate the conformational properties of fluorene molecules, starting with the identification of preferred conformations. The hybrid exchange-correlation functional, OPBE, and ZINDO/S-CI showed that each oligomer exhibits a tendency to adopt a specific chain arrangement, which could be distinguished by comparing their UV/vis electronic absorption and (13)C NMR spectra. This feature was used to identify the preferred conformation of the oligomer chains in chloroform-cast films by comparing experimental and theoretical UV/vis and (13)C NMR spectra. Moreover, the oligomer chain packing and dynamics in the films were studied by DSC and several solid-state NMR techniques, which indicated that the phase behavior of the films may be influenced by the tendency that each oligomeric chain has to adopt a given conformation.

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