No abstract

By simply doping the conventional light‐emitting polymer F8BT with a helically chiral aromatic molecule, it is shown that substantial levels of CP‐electroluminescence can be generated directly. Both photoluminescent and electroluminescent emission from the polymer are observed to become circularly polarized, with the sign of the CP emission directly determined by the handedness of the dopant.

Circularly polarized (CP) light is of interest in areas such as quantum optical computing, optical spintronics, biomedicine, and high efficiency displays. Direct emission of CP light from organic light-emitting diodes (OLEDs) has been a focus of research as it has the immediate application of increasing efficiency and simplifying device architecture in OLED based displays. High dissymmetry (gEL) factor values have been reported for devices employing fluorescent polymers, but these CP-OLEDs are limited in their ultimate efficiencies by the type of emissive electronic transitions involved. In contrast, phosphorescent OLEDs (PHOLEDs) can emit light from triplet excited states and can therefore achieve very high efficiencies. However, CP-PHOLEDs are significantly understudied, and the two previous reports suffered from very low brightness or gEL values. Here, we use a platinahelicene complex to construct a CP-PHOLED that achieves both a display level brightness and a high gEL factor. The dissymmetry of CP emission reached with this proof-of-concept single-layer helicene-based device is sufficient to provide real-world benefits over nonpolarized emission and paves the way toward chiral metal complex-based CP-PHOLED displays.

The emission of circularly-polarized light is central to many applications, including data storage, quantum computation, biosensing, environmental monitoring and display technologies. An emerging method to induce (chiral) circularly-polarized (CP) electroluminescence from the active layer of polymer light emitting diodes (polymer OLEDs; PLEDs) involves blending achiral polymers with chiral small molecule additives, where the handedness/sign of the CP light is controlled by the absolute stereochemistry of the small molecule. Through the in-depth study of such a system we report an interesting chiroptical property: the ability to tune the sign of CP light as function of active layer thickness for a fixed enantiomer of the chiral additive. We demonstrate that it is possible to achieve both efficient (4.0 cd/A) and bright (8000 cd/m 2) CP-PLEDs, with high dissymmetry of emission of both left handed (LH) and right handed (RH) light, depending on thickness (thin films, 110 nm: g EL = 0.51, thick films, 160 nm: g EL = −1.05, with the terms "thick" and "thin" representing the upper and lower limits of the thickness regime studied), for the same additive enantiomer. We propose that this arises due to an interplay between localized CP emission originating from molecular chirality and CP light amplification or inversion through a chiral medium. We link morphological, spectroscopic, and electronic characterization in thin films and devices with theoretical studies in an effort to determine the factors that underpin these observations. Through the control of active layer thickness and device architecture, this study provides insights into the mechanisms that result in CP luminescence from CP-PLEDs, opportunities in CP photonic device design, and demonstrate high performance CP-PLEDs.

Current–voltage, impedance, and transient conductance measurements have been carried out on indium-tin-oxide/poly(phenylene vinylene)/Al light emitting diodes. In these devices injection and transport is expected to be dominated by positive carriers. Fowler–Nordheim tunneling theory cannot account for the temperature dependence, the thickness dependence, or the current magnitude of the current–voltage characteristics. Space-charge limited current theory with an exponential distribution of traps is however in extremely good agreement with all of the recorded current–voltage results in the higher applied bias regime (approximately 0.7⩽V/d⩽1.6×106 V cm−1). This gives a trap density Ht of 5(±2)×1017 cm−3 and the product of μNHOMO of between 1014 and 5×1012 cm−1 V−1 s−1. Assuming NHOMO is 1020 cm−3 gives an effective positive carrier mobility between 10−6 and 5×10−8 cm2 V−1 s−1. The characteristic energy Et of the exponential trap distribution is 0.15 eV at higher temperatures (190⩽T⩽290 K), but this decreases as the devices are cooled, indicating that the distribution is in fact a much steeper function of energy closer to the highest occupied molecular orbital (HOMO) levels. The current–voltage characteristics in the lower applied bias regime (approximately V/d⩽0.7×106 V cm−1) can be fitted to pure space-charge limited current flow with a temperature and field dependent mobility of Arrhnenius form with a mobility at 290 K close to the above values. If NHOMO lies between 1021 and 1019 cm−3, then the trap filled limit bias gives a mobility independent value of Ht of 3(±1)×1017 cm−3. Capacitance–voltage measurements show that at zero bias the devices are fully depleted, and that the acceptor dopant density NA must be less than about 1016 cm−3. The impedance results show that the devices can be modeled on a single, frequency independent, parallel resistor-capacitor circuit with a small series resistor. The variation of the resistor and capacitor in the parallel circuit with applied bias and temperature are consistent with the space-charge limited current theory with the same exponential trap distribution used to model the current–voltage characteristics. Initial results for transient conductance measurements are reported. The transients have decay times greater than 300 s and exhibit a power-law dependence with time. This is shown to be exactly the behavior expected for the decay of an exponential trap distribution. Measurements at higher temperatures (290⩾T⩾150 K) give an Et of 0.15 eV, in excellent agreement with that found from the current–voltage measurements. This value of Et is exactly that found by similar analysis of the current–voltage characteristics in negative carrier dominated dialkoxy poly(phenylene vinylene) and Mq3 devices. It is proposed that this bulk transport dominated behavior is purely a consequence of hopping conduction through an approximately Gaussian density of states in which the deep sites act as traps.

Chiral molecules exist as pairs of nonsuperimposable mirror images; a fundamental symmetry property vastly underexplored in organic electronic devices. Here, we show that organic field-effect transistors (OFETs) made from the helically chiral molecule 1-aza[6]helicene can display up to an 80-fold difference in hole mobility, together with differences in thin-film photophysics and morphology, solely depending on whether a single handedness or a 1:1 mixture of left- and right-handed molecules is employed under analogous fabrication conditions. As the molecular properties of either mirror image isomer are identical, these changes must be a result of the different bulk packing induced by chiral composition. Such underlying structures are investigated using crystal structure prediction, a computational methodology rarely applied to molecular materials, and linked to the difference in charge transport. These results illustrate that chirality may be used as a key tuning parameter in future device applications

In this paper, electron transport of pure and DMC doped polyfluorne (PF) films have been studied at various doping concentrations. Pure films show space charge limited conduction with field and temperature dependent mobility. The J-V characteristics of doped PF were ohmic at low voltages due to thermally released carriers from dopant states. At higher voltages the current density increases nonlinearly due to field dependent mobility and carrier concentration thereby lling of tail states of HOMO of the host. The conductivity of doped fims were analyzed using the Unified Gaussian Disorder Model (UGDM). The carrier concentration obtained from the fitting show a non-linear dependence on doping concentration which may be due to a combined effect of thermally activated carrier generation and increased carrier mobility.

The origin of electrophosphorescence from a doped polymer light emitting diode ͑LED͒ has been investigated. A luminescent polymer host, poly͑9,9-dioctylfluorene͒ ͑PFO͒, was doped with a red phosphorescent dye, 2,3,7,8,12,13,17,18-octaethyl-21H,23H-porphyrin platinum͑II͒ ͑PtOEP͒. The maximum external quantum efficiency of 3.5% was obtained at a concentration of 4% PtOEP by weight. Energy transfer mechanisms between PFO and PtOEP were studied by absorption, photoluminescence, and photoinduced absorption spectroscopy. Even though electroluminescence spectra were dominated by PtOEP at a concentration of only 0.2 wt % PtOEP, Förster transfer of singlet excitons was weak and there was no evidence for Dexter transfer of triplet excitons. We conclude that the dominant emission mechanism in doped LED's is charge trapping followed by recombination on PtOEP molecules.