Electrical and Photoinduced Degradation of Polyfluorene Based Films and Light-Emitting Devices
TL;DR: Degradation-induced changes in the structural and optical properties of polyfluorene-based blue emitting films and LEDs are examined using spectroscopic (FTIR, UV−vis, photo- and electroluminescence), analytical (FT IR and ESCA), and scanning probe microscopy techniques.
Abstract: Degradation-induced changes in the structural and optical properties of the polyfluorene-based blue emitting films and LEDs are examined using spectroscopic (FTIR, UV−vis, photo- and electroluminescence), analytical (FTIR and ESCA), and scanning probe microscopy techniques. The materials studied are oligomers (DP ∼ 10) of 9,9-di-n-hexylfluorene and its random copolymer with anthracene. In situ FTIR monitoring is used to characterize chemical changes in the active layer of operating LED devices. Two primary mechanisms of degradation are identified. In the first, photooxidation of the polymer matrix leads to the formation of an aromatic ketone, most likely fluorenone at the chain terminating monomer units, which quenches the fluorescence. The second process promotes aggregate formation, which then leads to loss of luminous intensity by exciton transfer and relaxation through excimers.
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TL;DR: School of Chemistry, Bio21 Institute, University of Melbourne, 30 Flemington Road, Victoria 3010, Australia; School of Materials Science and Engineering, Nanyang Technological University, Nastyang Avenue, Republic of Singapore 639798; Institute of Materials Research and Engineering (IMRE) and the Agency for Science, Technology and Research (A*STAR), 3 Research Link, Singapore 117602.
Abstract: A review was presented to demonstrate a historical description of the synthesis of light-emitting conjugated polymers for applications in electroluminescent devices. Electroluminescence (EL) was first reported in poly(para-phenylene vinylene) (PPV) in 1990 and researchers continued to make significant efforts to develop conjugated materials as the active units in light-emitting devices (LED) to be used in display applications. Conjugated oligomers were used as luminescent materials and as models for conjugated polymers in the review. Oligomers were used to demonstrate a structure and property relationship to determine a key polymer property or to demonstrate a technique that was to be applied to polymers. The review focused on demonstrating the way polymer structures were made and the way their properties were controlled by intelligent and rational and synthetic design.
2,378 citations
TL;DR: A review about electroluminescence from organic materials and deals in detail with organic light-emitting diodes (OLEDs), lightemitting electrochemical cells (LECs) and electrogenerated chemilumi-nescence (ECL) reflecting different electrooptical appli-cations of conjugated materials as mentioned in this paper.
Abstract: This article provides a review about electroluminescence from organic materials and deals in detail with organic light-emitting diodes (OLEDs), light-emitting electro-chemical cells (LECs) and electrogenerated chemilumi-nescence (ECL) reflecting different electrooptical appli-cations of conjugated materials. It is written from an organic chemist's point of view and pays particular attention to the development of organic materials involved in corresponding devices. In recent years a substantial amount of both academic and industrial research has been directed to organic electroluminescence in an effort to improve the processability and tunability of organic materials and the longevity of OLEDs and LECs. On the eve of the commercialization of organic electrolumi-nescence this review provides an overview of lifetimes and efficiencies attained and reflects materials and device concepts developed over the last decade. In this context electrogenerated chemiluminescence is discussed with respect to its importance as a versatile tool to simulate the fundamental electrochemical processes in OLEDs.
1,657 citations
TL;DR: In this paper, the authors focus on reliable structure-property relationships regarding substitution pattern, solid state morphology, and optical/electronic properties, and the key role of degradation-induced keto defect sites in fluorerse-type polymers and strategies for obtaining defect-free polyfluorenes.
Abstract: Alkylsabstituted polyfluorenes have emerged as a very attractive class of conju gated polymers, especially for display applications, owing to their pure blue and efficient electroluminescence coupled with a high charge-carrier mobility and good processability. The availability of specific and highly regroselective coupling reactions provides a rich variety of taifored polyfluorene-type paly mers and copolymers. The focus of this review, therefore, is on reliable structure-property relationships regarding (i) the interplay of substitution pattern, solid state morphology, and optical/electronic properties, and (ii) the key role of degradation-induced keto defect sites in fluorerse-type polymers, and strategies for obtaining defect-free polyfluorenes.
1,557 citations
TL;DR: In this paper, a review of conjugated polymers with 1D and 2D topological structures is presented, and a design approach for the alternating donor-acceptor (D-A) copolymers is proposed.
668 citations
TL;DR: In this article, a structural model based on intrachain ordering was proposed to account for the changes of the absorption spectrum of poly(9,9-dioctylfluorene) (PFO) films under certain physicochemical treatment protocols.
Abstract: From photophysical evidence, we suggest a structural model based on intrachain ordering that can account for the changes of the absorption spectrum of poly(9,9-dioctylfluorene) (PFO) films under certain physicochemical treatment protocols. We correlate this model to the results of X-ray fiber diffraction experiments.
615 citations
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TL;DR: In this article, the authors demonstrate that poly(p-phenylene vinylene), prepared by way of a solution-processable precursor, can be used as the active element in a large-area light-emitting diode.
Abstract: CONJUGATED polymers are organic semiconductors, the semiconducting behaviour being associated with the π molecular orbitals delocalized along the polymer chain. Their main advantage over non-polymeric organic semiconductors is the possibility of processing the polymer to form useful and robust structures. The response of the system to electronic excitation is nonlinear—the injection of an electron and a hole on the conjugated chain can lead to a self-localized excited state which can then decay radiatively, suggesting the possibility of using these materials in electroluminescent devices. We demonstrate here that poly(p-phenylene vinylene), prepared by way of a solution-processable precursor, can be used as the active element in a large-area light-emitting diode. The combination of good structural properties of this polymer, its ease of fabrication, and light emission in the green–yellow part of the spectrum with reasonably high efficiency, suggest that the polymer can be used for the development of large-area light-emitting displays.
10,463 citations
TL;DR: In this article, the results of photoelectric cross-sections for the Kα lines of magnesium at 1254 eV and of aluminum at 1487 eV were given for Z values up to 96.
4,891 citations
TL;DR: In this paper, a summary of the various type cases for molecular dimers, trimers and double and triple molecules in the description of the molecular exciton strong-coupling model is presented.
Abstract: The molecular exciton model has received its most extensive development and application in the field of molecular crystals1'2. More recently, numerous applications to non-crystalline molecular composite systems have been made, including van der Waals and hydrogen-bonded dimers, trimers, and higher order aggregates. Another type of composite system has also been investigated, namely the composite molecule consisting of covalently bonded molecular units, with intrinsic individual unsaturated electronic systems so isolated by single bonds that but little or insignificant electronic overlap between units may occur. It is now well established that in molecular aggregates and in composite molecules, exciton effects may be observed if sufficiently strong electronic transitions exist in the component sub-units. The result of exciton splitting of excited states in the composite molecule may be the appearance of strong spectral shifts or splittings (which may be of the order of 2000 cm—1) of the absorption bands for the component molecules. At the same time, as a consequence of the exciton splitting of the excited state manifold, an enhancement of triplet state excitation may result. The purpose of this paper is to present a summary of the various type cases for molecular dimers, trimers and double and triple molecules in the description of the molecular exciton strong-coupling model. Then it will be shown by new experimental examples that, even in those cases where no significant exciton effect is observable in the singlet—singlet absorption spectrum for the composite molecule (intermediate and weak coupling cases), the enhancement of lowest triplet state excitation may still be conspicuous and significant. The ideas which are summarized in this paper have a curious history. Long ago, Kautsky and Merkel3 demonstrated experimentally that aggregation of dyes facilitated their action as photophysical sensitizers in photochemical reactions, at the same time diminishing their fluorescence efficiency. Kautsky attributed these easily demonstrated effects to enhancement of metastable state excitation in the aggregate dye. There is no doubt today that the metastable state he described is the lowest triplet state of the molecules studied. However, he did not distinguish between intrinsic and enhanced metastable (triplet) state excitation, so his interpretations were largely overlooked. Forster in l946 used the quasi-classical vector model to
3,597 citations
TL;DR: In this article, the authors reported visible light emission from Shottky diodes made from semiconducting polymers, confirming the discovery by the Cambridge group [Nature 347, 539 (1990)].
Abstract: We report visible light emission from Shottky diodes made from semiconducting polymers, confirming the discovery by the Cambridge group [Nature 347, 539 (1990)]. Our results demonstrate that light‐emitting diodes can be fabricated by casting the polymer film from solution with no subsequent processing or heat treatment required. Electrical characterization reveals diode behavior with rectification ratios greater than 104. We propose that tunneling of electrons from the recitifying metal contact into the gap states of the positive polaron majority carriers dominates current flow and provides the mechanism for light emission.
2,038 citations