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    ABSTRACT: The effect of a commonly used hole injection layer, poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT–PSS), on polymer light-emitting diode (PLED) performance has been investigated. A series of four different types of commercial PEDOT–PSS, with varying resistivity and work function were examined in devices with the structure Indium Tin Oxide (ITO)/PEDOT–PSS/High Molecular Weight Poly(n-vinylcarbazole) (PVKH): 30% N,N′-bis(3-methylphenyl)-N,N′-diphenylbenzidine (TPD)/Low molecular Weight Poly(n-vinylcarbazole) (PVKL): 40% 2-(4-Biphenyl)-5-(4-tert-butylphenyl)-1,2,4-oxadiazole (PBD): 8% Ir(ppy)3. It was found that the PEDOT–PSS with the highest work function and resistivity produced the devices with the highest efficiencies; this is due to the improved hole injection effect, the decrease in electron leakage current and the prevention of pixel crosstalk. A maximum device current efficiency of 33.4 cd A−1 has been achieved for the most resistive PEDOT; this corresponded to an external quantum efficiency (E.Q.E.) of 11%. Increasing the work function of the PEDOT used resulted in a 60% increase in E.Q.E. and device efficiency for PEDOTs in the same resistivity range. Drift–diffusion simulations, carried out using SEmiconducting Thin Film Optics Simulation software (SETFOS) 3.2, produced J–V curves in good agreement with the experimentally observed results; this allowed us to extract qualitative values for the effective device mobility along with the PEDOT work function and resistivity.
    Organic Electronics 01/2014; 15(1):245–250.
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    ABSTRACT: The absolute density of SD radicals in a supersonic jet has been measured down to (1.1 ± 0.1) × 10(5) cm(-3) in a modestly specified apparatus that uses a cross-correlated combination of cavity ring-down and laser-induced fluorescence detection. Such a density corresponds to 215 ± 21 molecules in the probe volume at any given time. The minimum detectable absorption coefficient was quantum-noise-limited and measured to be (7.9 ± 0.6) × 10(-11) cm(-1), in 200 s of acquisition time, corresponding to a noise-equivalent absorption sensitivity for the apparatus of (1.6 ± 0.1) × 10(-9) cm(-1) Hz(-1/2).
    Physical Chemistry Chemical Physics 10/2013;
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    ABSTRACT: Nickel nanoparticles have been created in an organic-based matrix by the reaction of Ni(COD)2 (COD = 1,5-bis-cyclooctadiene) and 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (TCNQF4). The size of the nickel nanoparticles can be controlled by the use of different solvents and inclusion of tetrahydrofuran (THF) within the reaction to stabilise the Ni(0) atoms from the Ni(COD)2. Materials are characterised with a combination of X-ray diffraction, electron microscopy and magnetometry and it is found that samples made using a halocarbon solvent resulted in clustered bulk Ni particles (size ≤ 10 nm) with anomalously high superparamagnetic blocking temperatures. Using an isocyanide solvent produces smaller (size ∼ 1 nm), well dispersed particles that show little evidence of superparamagnetic blocking in the range of temperatures investigated (>2 K). In all samples there is another component which dominates the magnetic response at low temperatures and shows an interesting temperature dependent scaling behaviour when plotted as M vs. B/T which we believe is related to the organo-metallic matrix that the particles are trapped within. We propose that the enhanced blocking temperature of particles synthesised using halocarbon solvents can be attributed to inter-particle dipolar interactions and nanoparticle-matrix exchange interactions.
    Nanoscale 10/2013;
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    ABSTRACT: We demonstrate a nonequilibrium phase transition in a dilute thermal atomic gas. The phase transition, between states of low and high Rydberg occupancy, is induced by resonant dipole-dipole interactions between Rydberg atoms. The gas can be considered as dilute as the atoms are separated by distances much greater than the wavelength of the optical transitions used to excite them. In the frequency domain, we observe a mean-field shift of the Rydberg state which results in intrinsic optical bistability above a critical Rydberg number density. In the time domain, we observe critical slowing down where the recovery time to system perturbations diverges with critical exponent α=-0.53±0.10. The atomic emission spectrum of the phase with high Rydberg occupancy provides evidence for a superradiant cascade.
    Physical Review Letters 09/2013; 111(11):113901.
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    ABSTRACT: Organic light-emitting diodes (OLEDs) have their performance limited by the number of emissive singlet states created upon charge recombination (25%). Recently, a novel strategy has been proposed, based on thermally activated up-conversion of triplet to singlet states, yielding delayed fluorescence (TADF), which greatly enhances electroluminescence. The energy barrier for this reverse intersystem crossing mechanism is proportional to the exchange energy (ΔEST ) between the singlet and triplet states; therefore, materials with intramolecular charge transfer (ICT) states, where it is known that the exchange energy is small, are perfect candidates. However, here it is shown that triplet states can be harvested with 100% efficiency via TADF, even in materials with ΔEST of more than 20 kT (where k is the Boltzmann constant and T is the temperature) at room temperature. The key role played by lone pair electrons in achieving this high efficiency in a series of ICT molecules is elucidated. The results show the complex photophysics of efficient TADF materials and give clear guidelines for designing new emitters.
    Advanced Materials 05/2013;
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    ABSTRACT: Bright solitons are non-dispersive wave solutions, arising in a diverse range of nonlinear, one-dimensional systems, including atomic Bose-Einstein condensates with attractive interactions. In reality, cold-atom experiments can only approach the idealized one-dimensional limit necessary for the realization of true solitons. Nevertheless, it remains possible to create bright solitary waves, the three-dimensional analogue of solitons, which maintain many of the key properties of their one-dimensional counterparts. Such solitary waves offer many potential applications and provide a rich testing ground for theoretical treatments of many-body quantum systems. Here we report the controlled formation of a bright solitary matter-wave from a Bose-Einstein condensate of (85)Rb, which is observed to propagate over a distance of ∼1.1 mm in 150 ms with no observable dispersion. We demonstrate the reflection of a solitary wave from a repulsive Gaussian barrier and contrast this to the case of a repulsive condensate, in both cases finding excellent agreement with theoretical simulations using the three-dimensional Gross-Pitaevskii equation.
    Nature Communications 05/2013; 4:1865.
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    ABSTRACT: Glassy polymers show "strain hardening": at constant extensional load, their flow first accelerates, then arrests. Recent experiments under such loading have found this to be accompanied by a striking dip in the segmental relaxation time. This can be explained by a minimal nonfactorable model combining flow-induced melting of a glass with the buildup of stress carried by strained polymers. Within this model, liquefaction of segmental motion permits strong flow that creates polymer-borne stress, slowing the deformation enough for the segmental (or solvent) modes then to re-vitrify. Here, we present new results for the corresponding behavior under step-stress shear loading, to which very similar physics applies. To explain the unloading behavior in the extensional case requires introduction of a "crinkle factor" describing a rapid loss of segmental ordering. We discuss in more detail here the physics of this, which we argue involves non-entropic contributions to the polymer stress, and which might lead to some important differences between shear and elongation. We also discuss some fundamental and possibly testable issues concerning the physical meaning of entropic elasticity in vitrified polymers. Finally, we present new results for the startup of steady shear flow, addressing the possible role of transient shear banding.
    The Journal of Chemical Physics 03/2013; 138(12):12A504.
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    ABSTRACT: Printable electronics is an innovative area of technology with great commercial potential. Here, a screen-printed functional ink, comprising a combination of semiconducting acicular particles, electrically insulating nanoparticles and a base polymer ink, is described that exhibits pronounced pressure sensitive electrical properties for applications in sensing and touch sensitive surfaces. The combination of these components in the as-printed ink yield a complex structure and a large and reproducible touch pressure sensitive resistance range. In contrast to the case for some composite systems, the resistance changes occur down to applied pressures of 13 Pa. Current-voltage measurements at fixed pressures show monotonic non-linear behaviour, which becomes more Ohmic at higher pressures and in all cases shows some hysteresis. The physical basis for conduction, particularly in the low pressure regime, can be described in terms of field assisted quantum mechanical tunnelling.
    Nanotechnology 03/2013; 24(16):165501.
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    ABSTRACT: We use a microwave field to control the quantum state of optical photons stored in a cold atomic cloud. The photons are stored in highly excited collective states (Rydberg polaritons) enabling both fast qubit rotations and control of photon-photon interactions. Through the collective read-out of these pseudospin rotations it is shown that the microwave field modifies the long-range interactions between polaritons. This technique provides a powerful interface between the microwave and optical domains, with applications in quantum simulations of spin liquids, quantum metrology and quantum networks.
    Physical Review Letters 03/2013; 110(10):103001.
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    ABSTRACT: We study theoretically the onset of shear banding in the three most common time-dependent rheological protocols: step stress, finite strain ramp (a limit of which gives a step strain), and shear startup. By means of a linear stability analysis we provide a fluid-universal criterion for the onset of banding for each protocol, which depends only on the shape of the experimentally measured time-dependent rheological response function, independent of the constitutive law and internal state variables of the particular fluid in question. Our predictions thus have the same highly general status, in these time-dependent flows, as the widely known criterion for banding in steady state (of negatively sloping shear stress vs shear rate). We illustrate them with simulations of the Rolie-Poly model of polymer flows, and the soft glassy rheology model of disordered soft solids.
    Physical Review Letters 02/2013; 110(8):086001.
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