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A series of novel arylene ladder polymers incorporating conjugated 1,5- and 2,6-naphthylene building blocks were synthesized. The polyketone ladder polymer precursors were prepared via a palladium-mediated Suzuki-type cross- coupling reaction using both conventional and microwave heating. While the 2,6-naphthylene polyketone precursor (2,6- NPK) was accessible from both heating protocols. the 1,5-naphthylene linked polyketones were only accessible via microwave-assisted (uW) procedures. and the polymer 1,5-NLP2 is the first example of a ladder polymer consisting exclusively of alternating six-membered rings prepared from this reaction sequence. The solution optical spectra of the final naphthylene ladder polymers exhibit the characteristic spectral shapes with a steep absorption edge and a vibronic fine structure common to fully rigidified ladder structures. The structural modification of the substitution pattern and the linkage positions at the naphthylene unit allows some tuning of the absorption and emission bands of the ladder polymers. The 2,6-naphthylene derivative exhibits an intense blue photoluminescence, while the two 1,5-naphthylene- linked ladder polymers exhibit a red shift of the 0-0 electronic transitions, leading to a blue-green photoluminescence
It is well known that the performance of solar cells based on a blend of hole-accepting and electron-accepting conjugated polymers as the active material depend crucially on the length scale of the resulting phase separated morphology. However, a direct control of this morphology is difficult if the layer is prepared from an organic solvent. To circumvent this difficulty, recently a universal method to fabricate defined nano-structured blend layer using nanoparticles dispersed in water was demonstrated. These nanoparticles were prepared with the miniemulsion method, which allows for the preparation of semiconducting polymer nanospheres (SPNs) with diameters in the range of 30 to 300 nanometres. Since the process starts from the active material dissolved in a common solvent, it can be applied to the fabrication of nanoparticles of blends of polymers with oligomers or even with inorganic materials. We present here for the first time scanning near field optical microscopy (SNOM) investigations on these novel nanostructured polymer layers. We show that by spin-coating a mixture of two different dispersions a nanoparticle monolayer with a statistically distribution of the nanoparticles can be obtained. Mixing conjugated polymer nanoparticles with some inert particles like polystyrene beads may allow for the preparation of nano-sized light emitters
An increase in random molecular vibrations of a solid owing to heating above the melting point leads to a decrease in its long-range order and a loss of structural symmetry. Therefore conventional liquids are isotropic media. Here we report on a light-induced isothermal transition of a polymer film from an isotropic solid to an anisotropic liquid state in which the degree of mechanical anisotropy can be controlled by light. Whereas during irradiation by circular polarized light the film behaves as an isotropic viscoelastic fluid, it shows considerable fluidity only in the direction parallel to the light field vector under linear polarized light. The fluidization phenomenon is related to photoinduced motion of azobenzene-functionalized molecular units, which can be effectively activated only when their transition dipole moments are oriented close to the direction of the light polarization. We also describe here how the photofluidization allows nanoscopic elements of matter to be precisely manipulated
We present a flashlamp-pumped Nd: YAG laser simultaneously emitting pulse structures on microsecond, nanosecond and picosecond time scales. Within a microsecond flashlamp pump pulse a nonlinear reflector based on stimulated Brillouin scattering (SBS) generates several Q-switch pulses. The phase-conjugating effect of the SBS reflector provides a compensation of phase distortions generated inside the laser rod, resulting in transverse fundamental mode operation. Additional acousto-optic loss modulation inside the resonator leads to mode locking. As a result, each Q-switch pulse is subdivided into several picosecond pulses. Energies of up to 2 mJ for the mode-locked pulses with durations between 220 and 800 ps are demonstrated. The wide variability of the laser's temporal output parameters as well as its high beam quality make it a splendid tool for fundamental research in laser materials processing
The existing optical microscopes form an image by collecting photons emitted from an object. Here we report on the experimental realization of microscopy without the need for direct optical communication with the sample. To achieve this, we have scanned a single gold nanoparticle acting as a nanoantenna in the near field of a sample and have studied the modification of its intrinsic radiative properties by monitoring its plasmon spectrum
We re-assess expected properties of the presumed dust belt of Mars formed by impact ejecta from Deimos. Previous studies have shown that dynamics of Deimos particles are dominated by two perturbing forces: radiation pressure (RP) and Mars' oblateness (J2). At the same time, they have demonstrated that lifetimes of particles, especially of grains about ten of micrometers in size, may reach more than 10(4) years. On such timescales, the Poynting-Robertson drag (PR) becomes important. Here we provide a study of the dynamics under the combined action of all three perturbing forces. We show that a PR decay of the semimajor axes leads to an adiabatic decrease of amplitudes and periods of oscillations in orbital inclinations predicted in the framework of the underlying RP+J2 problem. Furthermore, we show that smallest of the long-lived Deimos grains (radius approximate to 5-10 mum) may reach a chaotic regime, resulting in unpredictable and abrupt changes of their dynamics. The particles just above that size (approximate to 10- 15 mum) should be the most abundant in the Deimos torus. Our dynamical analysis, combined with a more accurate study of the particle lifetimes, provides corrections to earlier predictions about the dimensions and geometry of the Deimos torus. In addition to a population, appreciably inclined and shifted towards the Sun, the torus should contain a more contracted, less asymmetric, and less tilted component between the orbits of Phobos and Deimos. (C) 2004 Elsevier Ltd. All rights reserved
Dielectric properties of zinc phthalocyanine thin films : effects of annealing in air and in N-2
(2005)
This work presents the effects of ambient conditions, in particular oxygen and humidity, on the dielectric spectra of thin zinc phthalocyanine (ZnPc) films equipped with interdigitated electrodes and the effect of annealing in dry N-2 or in ambient air. The measurements were performed in the frequency range 10(-2)-10(5) Hz. The results indicate that the electric properties of ZnPc films are not only affected by oxygen but also by water vapour the presence of which always leads to the drop in alternating current conductance (ac-conductance). Moreover, at room temperature, the ac-conductance of ZnPc films previously exposed to air exhibits a reversible change with humidity, which makes these films attractive for humidity sensing applications. (C) 2004 Elsevier B.V. All rights reserved
In this paper we report on time dependent configuration interaction singles (TD-CIS) calculations aimed at simulating two-photon-photoelectron emission (2PPE) spectra of metal films, the latter treated within a one-dimensional jellium model. The method is based on a many-electron approach in which electron-electron-scattering is approximately accounted for and no artificial lifetimes have to be assumed for excited electrons. This contrasts with one-electron models where lifetimes and "dissipation" have to be introduced. The driving force for the photoelectron ejection in 2PPE experiments is the electric field of two laser pulses that are generally separated by a delay time, Delta t. To compute energy- and time-resolved 2PPE signals P(E, Delta t), a new scheme based on the time-energy method is proposed to analyze electronic wave packets in asymptotic regions of the potential
The wave-guided travelling-wave laser action (amplified spontaneous emission) of a neat film of poly(p- phenylenevinylene) (PPV) on a quartz glass substrate prepared by a sulfinyl precursor technique is studied. The samples are transversally pumped with picosecond excitation pulses (wavelength 347.15 nm, duration 35 ps). Lasing occurs at 550 nm. The optical constants of the neat films are determined by transmittance measurements exploiting the multiple beam interference in the transparency region. A fluorescence spectroscopic characterisation is carried out determining the fluorescence quantum distribution, fluorescence quantum yield, degree of fluorescence polarisation, and fluorescence lifetime. The emitting chromophore size (emitting singlet exciton extension) is determined by the ratio of exciton radiative lifetime to repeat-unit based radiative lifetime. The obtained size of about two repeat units is discussed in a disordered solid-state polymer model
We establish strict upper limits for the Casimir interaction between multilayered structures of arbitrary dielectric or diamagnetic materials. We discuss the appearance of different power laws due to frequency-dependent material constants. Simple analytical expressions are in good agreement with numerical calculations based on Lifshitz theory. We discuss the improvements required for current ( meta) materials to achieve a repulsive Casimir force
We develop an effective low-frequency theory of the electromagnetic field in equilibrium with thermal objects. The aim is to compute thermal magnetic noise spectra close to metallic microstructures. We focus on the limit where the material response is characterised by the electric conductivity. At the boundary between empty space and metallic microstructures, a large jump occurs in the dielectric function which leads to a partial screening of low-frequency magnetic fields generated by thermal current fluctuations. We resolve a, discrepancy between two approaches used in the past to compute magnetic field noise spectra close to microstructured materials
[1] According to the well-known Coulomb failure criterion the variation of either stress or pore pressure can result in earthquake rupture. Aftershock sequences characterized by the Omori law are often assumed to be the consequence of varying stress, whereas earthquake swarms are thought to be triggered by fluid intrusions. The role of stress triggering can be analyzed by modeling solely three-dimensional (3-D) elastic stress changes in the crust, but fluid flows which initiate seismicity cannot be investigated without considering complex seismicity patterns resulting from both pore pressure variations and earthquake-connected stress field changes. We show that the epidemic-type aftershock sequence (ETAS) model is an appropriate tool to extract the primary fluid signal from such complex seismicity patterns. We analyze a large earthquake swarm that occurred in 2000 in Vogtland/NW Bohemia, central Europe. By fitting the stochastic ETAS model, we find that stress triggering is dominant in creating the observed seismicity patterns and explains the observed fractal interevent time distribution. External forcing, identified with pore pressure changes due to fluid intrusion, is found to directly trigger only a few percent of the total activity. However, temporal deconvolution indicates that a pronounced fluid signal initiated the swarm. These results are confirmed by our analogous investigation of model simulations in which earthquakes are triggered by fluid intrusion as well as stress transfers on a fault plane embedded in a 3-D elastic half-space. The deconvolution procedure based on the ETAS model is able to reveal the underlying pore pressure variations
X-ray diffraction by a crystal in a permanent external electric field : general considerations
(2005)
The variations of X-ray diffraction intensities from a crystal in the presence of a permanent external electric field is modeled analytically using a first-order stationary perturbation theory. The change in a crystal, induced by an external electric field, is separated into two contributions. The first one is related to a pure polarization of an electron subsystem, while the second contribution can be reduced to the displacements of the rigid pseudoatoms from their equilibrium positions. It is shown that a change of the X-ray diffraction intensities mainly originates from the second contribution, while the influence of the pure polarization of a crystal electron subsystem is negligibly small. The quantities restored from an X-ray diffraction experiment in the presence of an external electric field were analyzed in detail in terms of a rigid pseudoatomic model of electron density and harmonic approximation for the atomic thermal motion. Explicit relationships are derived that link the properties of phonon spectra with E-field-induced variations of a structure factor, pseudoatomic displacements and piezoelectric strains. The displacements can be numerically estimated using a model of independent atomic motion if the Debye - Waller factors and pseudoatomic charges are known either from a previous single-crystal X-ray diffraction study or from density functional theory calculations. The above estimations can be used to develop an optimum strategy for a data collection that avoids the measurements of reflections insensitive to the electric-field-induced variations
We study the stability of self-sustained oscillations under the influence of external noise. For small-noise amplitude a phase approximation for the Langevin dynamics is valid. A stationary distribution of the phase is used for an analytic calculation of the maximal Lyapunov exponent. We demonstrate that for small noise the exponent is negative, which corresponds to synchronization of oscillators. (c) 2004 Elsevier B.V. All rights reserved
We study Hamiltonian chaos generated by the dynamics of passive tracers moving in a two-dimensional fluid flow and describe the complex structure formed in a chaotic layer that separates a vortex region from the shear flow. The stable and unstable manifolds of unstable periodic orbits are computed. It is shown that their intersections in the Poincare map as an invariant set of homoclinic points constitute the backbone of the chaotic layer. Special attention is paid to the finite time properties of the chaotic layer. In particular, finite time Lyapunov exponents are computed and a scaling law of the variance of their distribution is derived. Additionally, the box counting dimension as an effective dimension to characterize the fractal properties of the layer is estimated for different duration times of simulation. Its behavior in the asymptotic time limit is discussed. By computing the Lyapunov exponents and by applying methods of symbolic dynamics, the formation of the layer as a function of the external forcing strength, which in turn represents the perturbation of the originally integrable system, is characterized. In particular, it is shown that the capture of KAM tori by the layer has a remarkable influence on the averaged Lyapunov exponents. (C) 2004 Elsevier Ltd. All rights reserved
We introduce a new survey of massive stars in the Galaxy and the Magellanic Clouds using the Fibre Large Array Multi- Element Spectrograph ( FLAMES) instrument at the Very Large Telescope ( VLT). Here we present observations of 269 Galactic stars with the FLAMES- Giraffe Spectrograph ( R similar or equal to 25 000), in fields centered on the open clusters NGC3293, NGC4755 and NGC6611. These data are supplemented by a further 50 targets observed with the Fibre- Fed Extended Range Optical Spectrograph ( FEROS, R = 48 000). Following a description of our scientific motivations and target selection criteria, the data reduction methods are described; of critical importance the FLAMES reduction pipeline is found to yield spectra that are in excellent agreement with less automated methods. Spectral classifications and radial velocity measurements are presented for each star, with particular attention paid to morphological peculiarities and evidence of binarity. These observations represent a significant increase in the known spectral content of NGC3293 and NGC4755, and will serve as standards against which our subsequent FLAMES observations in the Magellanic Clouds will be compared
In this Letter, the problem of finding optimal success probabilities of linear optics quantum gates is linked to the theory of convex optimization. It is shown that by exploiting this link, upper bounds for the success probability of networks realizing single-mode gates can be derived, which hold in generality for postselected networks of arbitrary size, any number of auxiliary modes, and arbitrary photon numbers. As a corollary, the previously formulated conjecture is proven that the optimal success probability of a nonlinear sign shift without feedforward is 1/4, a gate playing the central role in the scheme of Knill-Laflamme-Milburn for quantum computation. The concept of Lagrange duality is shown to be applicable to provide rigorous proofs for such bounds, although the original problem is a difficult nonconvex problem in infinitely many objective variables. The versatility of this approach is demonstrated
This contribution reports the combined influences of odd-even effects and the specific positioning of alkoxy side chains OR1 = (OCn+H-10(2(n+10)+1)) and OR2 = (OCnH2n+1) (with n = 6, 7, 8, 9) on the phenylene-ethynylene and phenylene- vinylene segments, respectively, on the optical properties of hybrid polymers P(n+10)/n of general repeating unit: -Ph-C equivalent to C-Ph-C equivalent to C-Ph-CH=CH-Ph-CH=CH-. For the polymeric materials, visual color impression varies alternatively between orange red (P16/6 and P18/8) and yellow (P17/7 and P19/9) according to the odd and even features of the alkoxy side chains, where odd or even relates to the total number of sp(3)-hybridized atoms within the side chains. This side chain related effect is ascribed to both absorptive and emissive behaviors of the polymers on the basis of photophysical investigations in the bulk. Almost identical thin film absorption spectra were obtained for all four materials; however, the photoluminescence of the odd polymers, P16/6 (lambda(f) = 556 nm) and P18/ 8 (lambda(f) = 614 nm), was red-shifted relative to that of their even counterparts (lambda(f) = 535 nm). Further, the P18/8 maximum at 614 nm can be readily assigned to excimer emission, as evidenced by the largest Stokes shift (5600 cm(- 1)), largest fwhmf-value (3700 cm(-1))(,) and the lowest Phi(f)-value of 24%. The strong pi-pi interchain interaction in P18/8, due to loose alkoxy side chains packing, does not only favor fluorescence quenching but also enable an effective inter- as well as intra-molecular recombination of the generated positive and negative polarons in electrolurninescence, which explains the good EL properties of this polymer irrespective of the solvent used. A voltage-dependent blue shift of the EL spectra of up to 100 nm was observed for P18/8 devices prepared from aromatic solvents. This red to green EL shift as observed with increasing voltage is assigned to conformational changes of the polymer chains with increasing temperature