Leonidas C. Palilis

Highly efficient molecular organic light-emitting diodes based on exciplex emission

Highly efficient exciplex emission is observed from molecular organic light-emitting diodes (MOLEDs) based on silole derivatives as emissive and electron transport materials, and a hole transporting amine derivative. A silole derivative, 2,5-di-(3-biphenyl)-1,1-dimethyl- 3,4-diphenylsilacyclopentadiene (PPSPP), which shows blue fluorescence (476 nm) with a high solid-state photoluminescence quantum yield of 85% was used as the emitter. Another silole derivative, 2,5-bis-(2′,2″-bipyridin-6-yl)-1,1-dimethyl-3,4-diphenylsilacyclopentadiene which exhibits high electron mobility, was used as the electron transport material. MOLEDs using these two siloles and N,N′-diphenyl-N,N′-(2-napthyl)-(1,1′-phenyl)-4,4′-diamine (NPB) as the hole transporter show electroluminescence (EL) emission centered at 495 nm. This red-shifted EL band relative to the blue fluorescence of PPSPP is assigned to a NPB:PPSPP exciplex. An operating voltage of 4.5 V was measured at 100u2009cd/m2 and an EL quantum efficiency of 3.4% was achieved ...

Determination of the width of the carrier recombination zone in organic light-emitting diodes

Bilayer organic light-emitting diodes based on tris-(8-hydroxyquinolinato) aluminum III have been fabricated where the thickness of the light-emitting layer was varied between 10 and 80 nm while maintaining a constant total thickness of the organic layers. The electroluminescence quantum efficiency of the devices was measured as a function of the emitter thickness, and used to determine the width of the carrier recombination zone at different electric fields. The width of the carrier recombination zone is found to decrease with an increase in electric field [from 70 nm (E=0.75 MV/cm) to 40 nm (E=1.0 MV/cm)]. It is also related to the field-dependent carrier injection efficiency. An estimate of the light output coupling factor (0.4) is also given based on this analysis.

Electron injection in "electron-only" devices based on a symmetric metal/silole/metal structure

We report on electron injection from two different metal electrodes into three silole derivatives, namely 2,5-di-(3-biphenyl)-1,1-dimethyl-3,4-diphenylsilacyclopentadiene (PPSPP), 1,2-bis(1-methyl-2,3,4,5,-tetraphenylsilacyclopentadienyl) ethane (2PSP) and 2,5-bis-(2, 2-bipyridin-6-yl)-1, 1-dimethyl-3,4-diphenylsilacyclopentadiene (PyPySPyPy), previously employed as emissive and electron transport materials in molecular organic light-emitting diodes (MOLEDs). Silole films were sandwiched between symmetric Mg:Ag or bilayer CsF-Al electrodes. The steady-state current density-voltage characteristics were measured as a function of the silole layer thickness for the two cathodes. The trap-free space-charge-limited current based on time-of-flight measurements compared with the injected electron current for PyPySPyPy indicated that Mg:Ag contacts limit the injected current, while CsF-Al contacts behave as quasi-ohmic contacts. Similar findings were obtained for 2PSP and PPSPP allowing steady-state derived electron mobility parameters to be extracted. Based on space-charge-limited conduction analysis of the measured current-voltage characteristics, PyPySPyPy is found to be a superior electron transporting silole with approximately an order of magnitude higher electron mobility (2.0/spl times/10/sup -4/ cm/sup 2//Vs) compared with those of 2PSP (2.4/spl times/10/sup -5/ cm/sup 2//Vs) and PPSPP (5.2/spl times/10/sup -5/ cm/sup 2//Vs), which is significantly higher than that of the prototype electron transport material tris (8-hydroxyquinolinolato) aluminum (III) (Alq/sub 3/) (6.5/spl times/10/sup -7/ cm/sup 2//Vs) at 0.6 MV/cm.

Energy transfer and excitation migration in a doped organic semiconductor

We have studied energy transfer to a dioxolane-substituted pentacene derivative, 6,14-bis-(triisopropylsilylethynyl)-1,3,9,11-tetraoxa-dicyclopenta[b,m]pentacene (TP-5), from tris(8-hydroxyquin-8-olinato) aluminum(III) (Alq3) by steady state and time-resolved photoluminescence (PL) spectroscopy. The Förster transfer radius is 27 Å, calculated from the fluorescence spectrum of Alq3 and the absorption spectrum of TP-5. We find that pentacene emission dominates the PL spectra of TP-5:Alq3 guest-host films, even at concentrations where the typical guest separation is significantly larger than the Förster transfer radius. Monte Carlo simulations of energy transfer to randomly dispersed guest molecules in the host matrix show that Förster-type energy transfer cannot completely account for the PL dynamics of the guest and host. Exciton diffusion within the Alq3 host followed by fluorescence of the host molecules or energy transfer to the guest explains the PL spectra and dynamics.

Efficient molecular organic light-emitting diodes based on silole derivatives

We report the performance of molecular organic light-emitting diodes (MOLEDs) using silole derivatives as emissive and electron transport materials. Two siloles, namely 2,5-di-(3-biphenyl)-1,1-dimethyl-3,4-diphenylsilacyclopentadiene (PPSPP) and 1,2-bis(1-methyl-2,3,4,5,-tetraphenylsilacyclopentadienyl)ethane (2PSP), with high PL quantum yields of 94% and 85%, respectively, were used as emissive materials. Another silole, namely 2,5-bis-(2,2-bipyridin-6-yl)-1,1-dimethyl-3,4-diphenylsilacyclopentadiene (PyPySPyPy), was used as the electron transport material. MOLEDs using these two siloles and NPB as the hole transport material show a low operating voltage of approximately 4.5 V at a luminance of 100 cd/m2 and high external electroluminescence (EL) quantum efficiencies of 3.4% and 3.8%, respectively, at 100 A/m2. MOLEDs based on PPSPP exhibit a red-shifted EL spectrum which is assigned to an exciplex formed at the PPSPP:NPB interface.

Polymer Electrodes for Flexible Organic Light-Emitting Devices

We report a high luminance and low operating voltage molecular organic light-emitting diode (MOLED) using a conducting polymer hole-injecting electrode (anode) on a plastic substrate. A dramatic improvement in the rectification ratio is observed upon the insertion of a buffer layer between the conducting polymer anode and the organic hole-transporting layer (HTL). Micro-shorts leading to a leakage current caused by the non-uniformity of the polymer film are greatly reduced. Atomic force microscope (AFM) images show a much smoother surface of the polymer anode/buffer layer relative to that of the bare polymer film. A slight increase (0.3eV ± 0.2eV) in the work function of the polymer anode upon the addition of the buffer layer is also measured. A simple method of patterning the conducting polymer electrode on various substrates including plastics is also reported. This approach conveniently provides finely patterned conducting polymer films with νm resolution while maintaining their intrinsic electrical and optical properties such as the surface sheet resistance and the optical transmittance.

Organic photovoltaic cells based on functionalized pentacenes

We report a study on solar cells using pentacene derivatives with triisopropylsilylethynyl substitution at the 6,13-position and 1,3-dioxolane substitution to the terminal benzenoid rings of pentacene as the electron donor and C60 as the electron acceptor. A significant increase in the open circuit voltage (Voc) was obtained in all the pentacene-derivative based cells with the highest Voc as high as 0.90 V, compared to a 0.24 V value for pentacene. The variation in the Voc of the cells is in qualitative agreement with the larger offset between ionization potential of the electron donor and the electron affinity of C60. The power conversion efficiency (η) at 100 mW/cm2 of EtTP-5/C60 cells reached 0.74%, which is comparable to that of a pentacene/C60 cell (0.82%).

High-efficiency silole-based molecular organic light-emitting devices using highly conducting polymer anode contacts

We present high efficiency and high luminance molecular organic light-emitting diodes (MOLEDs) using a conducting polymer as a hole-injecting electrode (anode), a CsF/Al bilayer as a cathode, and silole derivatives as an emitter and/or an electron transporter. The conducting polymer films, poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS), were either spin-cast from aqueous dispersions or pre-coated on plastic substrates (courtesy Agfa Gevaert N.V. Belgium). The surface sheet resistance of the conducting polymer films is in the range of 150Ohms/sq ~ 1500 Ohms/sq. MOLEDs fabricated with a low sheet resistance (150 Ohms/sq) conducting polymer as an anode without using an ITO underlayer and CsF/Al as a cathode exhibit very low operating voltages (4.5V @ 100 cd/m2 and 6.5V @ 1,000 cd/m2). This good device performance is attributable to the low sheet resistance of the conducting polymer anode and the high electron mobility of the silole derivative, namely 2,5-bis-(2,2-bipyridin-6-yl)-1,1-dimethyl-3,4-diphenylsilacyclopentadiene (PyPySPyPy), used as an electron transporter. Efficient electron injection from the CSF/Al cathode to the PyPySPyPy electron injection/transport layer also contributes to better charge balance and improved device efficiency.