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The formation of different micro- and nanostructures during the chemical synthesis of polypyrrole is reviewed shortly based on the conceptions of hard- and soft-templating models. Contrary to other models that emphasize the role of micelles it is found here that during the oxidative polymerization of pyrole using sulfonic acid dopants a crystalline hard template is found in the first steps of the reaction before the addition of the oxidant. This template is formed by a complex consisting of 2,5-bis(pyrrole-2-yl)pyrrolidine and the sulfonic acid anion. The acid catalyzed formation of this specific tripyrrole is discussed. (C) 2009 Elsevier B.V. All rights reserved.
We establish a quantitative relationship between the entanglement content of a single quantum chain at a critical point and the corresponding entropy of entanglement. We find that, surprisingly, the leading critical scaling of the single-copy entanglement with respect to any bipartitioning is exactly one-half of the entropy of entanglement, in a general setting of conformal field theory and quasifree systems. Conformal symmetry imposes that the single-copy entanglement scales as E-1(rho(L))=(c/6)ln L-(c/6)(pi(2)/ln L)+O(1/L), where L is the number of constituents in a block of an infinite chain and c denotes the central charge. This shows that from a single specimen of a critical chain, already half the entanglement can be distilled compared to the rate that is asymptotically available. The result is substantiated by a quantitative analysis for all translationally invariant quantum spin chains corresponding to all isotropic quasifree fermionic models. An example of the XY spin chain shows that away from criticality the above relation is maintained only near the quantum phase transition
We study theoretically the coherent and correlated motion of many fermions inside an infinite square well potential. We will look at electrons and He-3 atoms, which behave very differently not only because of their masses, but also because of their different interaction potential. Also, the level of theory and the role of approximations in the solution of the time-dependent Schrodinger equation will be discussed
We present two different approaches to detect and quantify phase synchronization in the case of coupled non- phase coherent oscillators. The first one is based on the general idea of curvature of an arbitrary curve. The second one is based on recurrences of the trajectory in phase space. We illustrate both methods in the paradigmatic example of the Rossler system in the funnel regime. We show that the second method is applicable even in the case of noisy data. Furthermore, we extend the second approach to the application of chains of coupled systems, which allows us to detect easily clusters of synchronized oscillators. In order to illustrate the applicability of this approach, we show the results of the algorithm applied to experimental data from a population of 64 electrochemical oscillators
We investigated the spectral properties of light-emitting diodes based on a deep blue-emitting pyrazoloquinoline dye doped into a poly(N-vinylcarbazole)-based matrix. Even though the electroluminescence (EL) of the host is redshifted and broadened with respect to the emission of the dye, the EL spectrum becomes fully dominated by the dye emission at concentrations of ca. 2 wt %. This is attributed to a competition of exciplex formation on the matrix and exciton formation on the dye.
Past studies have shown that the initiation of symbiosis between the Red-Sea soft coral Heteroxenia fuscescens and its symbiotic dinoflagellates occurs due to the chemical attraction of the motile algal cells to substances emanating from the coral polyps. However, the resulting swimming patterns of zooxanthellae have not been previously studied. This work examined algal swimming behaviour, host location and navigation capabilities under four conditions: (1) still water, (2) in still water with waterborne host attractants, (3) in flowing water, and (4) in flow with host attractants. Algae were capable of actively and effectively locating their host in still water as well as in flow. When in water containing host attractants, swimming became slower, motion patterns straighter and the direction of motion was mainly towards the host-even if this meant advancing upstream against flow velocities of up to 0.5 mm s(-1)supercript stop. Coral-algae encounter probability decreased the further downstream of the host algae were located, probably due to diffusion of the chemical signal. The results show how the chemoreceptive zooxanthellae modify their swimming pattern, direction, velocity, circuity and turning rate to accommodate efficient navigation in changing environmental conditions
Recent theoretical studies have shown contrasting effects of temporal correlation of environmental fluctuations ( red noise) on the risk of population extinction. It is still debated whether and under which conditions red noise increases or decreases extinction risk compared with uncorrelated ( white) noise. Here, we explain the opposing effects by introducing two features of red noise time series. On the one hand, positive autocorrelation increases the probability of series of poor environmental conditions, implying increasing extinction risk. On the other hand, for a given time period, the probability of at least one extremely bad year ("catastrophe") is reduced compared with white noise, implying decreasing extinction risk. Which of these two features determines extinction risk depends on the strength of environmental fluctuations and the sensitivity of population dynamics to these fluctuations. If extreme ( catastrophic) events can occur ( strong noise) or sensitivity is high ( overcompensatory density dependence), then temporal correlation decreases extinction risk; otherwise, it increases it. Thus, our results provide a simple explanation for the contrasting previous findings and are a crucial step toward a general understanding of the effect of noise color on extinction risk
We present a universal approach to the investigation of the dynamics in generalized models. In these models the processes that are taken into account are not restricted to specific functional forms. Therefore a single generalized models can describe a class of systems which share a similar structure. Despite this generality, the proposed approach allows us to study the dynamical properties of generalized models efficiently in the framework of local bifurcation theory. The approach is based on a normalization procedure that is used to identify natural parameters of the system. The Jacobian in a steady state is then derived as a function of these parameters. The analytical computation of local bifurcations using computer algebra reveals conditions for the local asymptotic stability of steady states and provides certain insights on the global dynamics of the system. The proposed approach yields a close connection between modelling and nonlinear dynamics. We illustrate the investigation of generalized models by considering examples from three different disciplines of science: a socioeconomic model of dynastic cycles in china, a model for a coupled laser system and a general ecological food web
The question as to whether state-selective population of molecular vibrational levels by shaped infrared laser pulses is possible in a condensed phase environment is of central importance for such diverse fields as time-resolved spectroscopy, quantum computing, or "vibrationally mediated chemistry." This question is addressed here for a model system, representing carbon monoxide adsorbed on a Cu(100) surface. Three of the six vibrational modes are considered explicitly, namely, the CO stretch vibration, the CO-surface vibration, and a frustrated translation. Optimized infrared pulses for state-selective excitation of "bright" and "dark" vibrational levels are designed by optimal control theory in the framework of a Markovian open-system density matrix approach, with energy flow to substrate electrons and phonons, phase relaxation, and finite temperature accounted for. The pulses are analyzed by their Husimi "quasiprobability" distribution in time-energy space.
Triplet energy back transfer in conjugated polymers with pendant phosphorescent iridium complexes
(2006)
The nature of Dexter triplet energy transfer between bonded systems of a red phosphorescent iridium complex 13 and a conjugated polymer, polyfluorene, has been investigated in electrophosphorescent organic light-emitting diodes. Red- emitting phosphorescent iridium complexes based on the [Ir(btp)2(acac)]fragment (where btp is 2-(2 '- benzo[b]thienyl)pyridinato and acac is acetylacetonate) have been attached either directly (spacerless) or through a - (CH2)(8)-chain (octamethylene-tethered) at the 9-position of a 9-octylfluorene host. The resulting dibromo- functionalized spacerless (8) or octamethylene-tethered (12) fluorene monomers were chain extended by Suzuki polycondensations using the bis(boronate)-terminated fluorene macromonomers 16 in the presence of end-capping chlorobenzene solvent to produce the statistical spacerless (17) and octamethylene-tethered ( 18) copolymers containing an even dispersion of the pendant phosphorescent fragments. The spacerless monomer 12 adopts a face-to-face conformation with a separation of only 3.6 angstrom between the iridium complex and fluorenyl group, as shown by X-ray analysis of a single crystal, and this facilitates intramolecular triplet energy transfer in the spacerless copolymers 17. The photo- and electroluminescence efficiencies of the octamethylene-tethered copolymers 18 are double those of the spacerless copolymers 17, and this is consistent with suppression of the back transfer of triplets from the red phosphorescent iridium complex to the polyfluorene backbone in 18. The incorporation of a -(CH2)(8)- chain between the polymer host and phosphorescent guest is thus an important design principle for achieving higher efficiencies in those electrophosphorescent organic light-emitting diodes for which the triplet energy levels of the host and guest are similar
We report that the performances of blue polymer electrophosphorescent devices are crucially depending on the choice of the electron transporting material incorporated into the emissive layer. Devices with 1,3-bis[(4-tert- butylphenyl)-1,3,4-oxidiazolyl]phenylene (OXD-7) doped at similar to 40 wt% into a poly(vinylcarbazole) matrix exhibited significantly higher efficiencies than those with 2-(4-biphenylyl)-5-(4-tert-butylphenyl)-1,3,4-oxadiazole (PBD), yielding maximum luminous and power efficiency values of 18.2 Cd/A and 8.8 lm/W, respectively. Time resolved photoluminescence measurements revealed a long lifetime phosphorescence component in layers with PBD, which we assign to significant triplet harvesting by this electron-transporting component. (c) 2006 American Institute of Physics
We study thermally induced birefringence in crystalline Nd:YAG zigzag slab lasers and the associated depolarization losses. The optimum crystallographic orientation of the zigzag slab within the Nd:YAG boule and photoelastic effects in crystalline Nd:YAG slabs are briefly discussed. The depolarization is evaluated using the temperature and stress distributions, calculated using a finite element model, for realistically pumped and cooled slabs of finite dimensions. Jones matrices are then used to calculate the depolarization of the zigzag laser mode. We compare the predictions with measurements of depolarization, and suggest useful criteria for the design of the gain media for such lasers.
High cw power using an external cavity for spectral beam combining of diode laser-bar emission
(2006)
In extension to known concepts of wavelength-multiplexing diode laser arrays, a new external cavity is presented. The setup simultaneously improves the beam quality of each single emitter of a standard 25 emitter broad-area stripe laser bar and spectrally superimposes the 25 beams into one. By using this external resonator in an "off-axis" arrangement, beam qualities of M-slow(2) < 14 and M-fast(2) < 3 with optical powers in excess of 10 W in cw operation are obtained.
We present a detailed, realistic analysis of the implementation of a proposal for a quantum phase gate based on atomic vibrational states, specializing it to neutral rubidium atoms on atom chips. We show how to create a double-well potential with static currents on the atom chips, using for all relevant parameters values that are achieved with present technology. The potential barrier between the two wells can be modified by varying the currents in order to realize a quantum phase gate for qubit states encoded in the atomic external degree of freedom. The gate performance is analyzed through numerical simulations; the operation time is similar to 10 ms with a performance fidelity above 99.9%. For storage of the state between the operations the qubit state can be transferred efficiently via Raman transitions to two hyperfine states, where its decoherence is strongly inhibited. In addition we discuss the limits imposed by the proximity of the surface to the gate fidelity.
In this Letter, we show that coherence and phase synchronization analysis are sensitive but not specific in detecting the correct class of underlying dynamics. We propose procedures to increase specificity and demonstrate the power of the approach by application to paradigmatic dynamic model systems. (c) 2006 Elsevier B.V. All rights reserved
An effective dynamical description of a general class of stochastic phase oscillators is presented. For this, the effective phase velocity is defined either by the stochastic phase oscillators invariant probability density or its first passage times. Using the first approach the effective phase exhibits the correct frequency and invariant distribution density, whereas the second approach models the proper phase resetting curve. The discrepancy of the effective models is most pronounced for noise-induced oscillations and is related to non-monotonicity of the stochastic phase variable due to fluctuations.
In this paper, a measuring technique is presented for the detection of radial oscillations of tube walls excited by changes in internal air pressure. On organ pipes, the oscillations were investigated by means of piezoelectric polymer films slightly tensioned around the pipe bodies. Employing sensors with patterned electrodes, the well-known elliptical oscillation of the cross section as well as an additional monopole breathing of the organ-pipe body were detected. For the monopole breathing, a close relationship between the pressure distribution of the air-column resonances inside the pipe and the circumference variations along the pipe was observed
Human comment is studied using data from 'tianya' which is one of the most popular on-line social systems in China. We found that the time interval between two consecutive comments on the same topic, called inter-event time, follows a power-law distribution. This result shows that there is no characteristic decay time on a topic. It allows for very long periods without comments that separate bursts of intensive comments. Furthermore, the frequency of a different ID commenting on a topic also follows a power-law distribution. It indicates that there are some "hubs" in the topic who lead the direction of the public opinion. Based on the personal comments habit, a model is introduced to explain these phenomena. The numerical simulations of the model fit well with the empirical results. Our findings are helpful for discovering regular patterns of human behavior in on-line society and the evolution of the public opinion on the virtual as well as real society.
The coherence length of the thermal electromagnetic field near a planar surface has a minimum value related to the nonlocal dielectric response of the material. We perform two model calculations of the electric energy density and the field's degree of spatial coherence. Above a polar crystal, the lattice constant gives the minimum coherence length. It also gives the upper limit to the near field energy density, cutting off its 1/z(3) divergence. Near an electron plasma described by the semiclassical Lindhard dielectric function, the corresponding length scale is fixed by plasma screening to the Thomas-Fermi length. The electron mean free path, however, sets a larger scale where significant deviations from the local description are visible
We develop an effective description of noise-induced oscillations based on deterministic phase dynamics. The phase equation is constructed to exhibit correct frequency and distribution density of noise-induced oscillations. In the simplest one-dimensional case the effective phase equation is obtained analytically, whereas for more complex situations a simple method of data processing is suggested. As an application an effective coupling function is constructed that quantitatively describes periodically forced noise-induced oscillations.
We report measurements on the synchronization properties of organ pipes. First, we investigate influence of an external acoustical signal from a loudspeaker on the sound of an organ pipe. Second, the mutual influence of two pipes with different pitch is analyzed. In analogy to the externally driven, or mutually coupled self-sustained oscillators, one observes a frequency locking, which can be explained by synchronization theory. Further, we measure the dependence of the frequency of the signals emitted by two mutually detuned pipes with varying distance between the pipes. The spectrum shows a broad '' hump '' structure, not found for coupled oscillators. This indicates a complex coupling of the two organ pipes leading to nonlinear beat phenomena.
Employing the chemically passive carbon reconstruction W(110)/C-R(15x3) as substrate for deposition of C-60 molecules, we have discovered by scanning tunneling microscopy two-dimensional self-assembly of fullerenes into uniform molecular nanoclusters with "magic" numbers. Our photoemission measurements determine van der Waals forces as the dominating interaction in this self-organizing two-dimensional molecular gas. Based on this, a theoretical determination of the cluster structures in the framework of the Girifalco model gives perfect agreement with the experiment
Ferroelectrets are thin films of polymer foams, exhibiting piezoelectric properties after electrical charging. Ferroelectret foams usually consist of a cellular polymer structure filled with air. Polymer-air composites are elastically soft due to their high air content as well as due to the size and shape of the polymer walls. Their elastically soft composite structure is one essential key for the working principle of ferroelectrets, besides the permanent trapping of electric charges inside the polymer voids. The elastic properties allow large deformations of the electrically charged voids. However, the composite structure can also possibly limit the stability and consequently the range of applications because of, e. g., penetration of gas and liquids accompanied by discharge phenomena or because of a mechanical pre-load which may be required during the application. Here, we discuss various stability aspects related to the piezoelectric properties of polypropylene ferroelectrets. Near and below room temperature, the piezoelectric effect and the stability of the trapped charges are practically independent from humidity during long-time storage in a humid atmosphere or water, or from operating conditions, such as continuous mechanical excitation. Thermal treatment of cellular polypropylene above -10 degrees C leads to a softening of the voided structure which is apparent from the decreasing values of the elastic modulus. This decrease results in an increase of the piezoelectric activity. Heating above 60 degrees C, however, leads to a decrease in piezoelectricity
Superexponential droplet fractalization as a hierarchical formation of dissipative compactons
(2010)
We study the dynamics of a thin film over a substrate heated from below in a framework of a strongly nonlinear one-dimensional Cahn-Hilliard equation. The evolution leads to a fractalization into smaller and smaller scales. We demonstrate that a primitive element in the appearing hierarchical structure is a dissipative compacton. Both direct simulations and the analysis of a self-similar solution show that the compactons appear at superexponentially decreasing scales, which means vanishing dimension of the fractal.
We report time-dependent configuration interaction singles calculations for the ultrafast laser driven many- electron dynamics in a polyatomic molecule, N-methyl-6-quinolone. We employ optimal control theory to achieve a nearly state-selective excitation from the S-0 to the S-1 state, on a time scale of a few (approximate to 6) femtoseconds. The optimal control scheme is shown to correct for effects opposing a state-selective transition, such as multiphoton transitions and other, nonlinear phenomena, which are induced by the ultrashort and intense laser fields. In contrast, simple two-level pi pulses are not effective in state-selective excitations when very short pulses are used. Also, the dependence of multiphoton and nonlinear effects on the number of states included in the dynamical simulations is investigated.
The concept of complementarity, originally defined for non-commuting observables of quantum systems with states of non-vanishing dispersion, is extended to classical dynamical systems with a partitioned phase space. Interpreting partitions in terms of ensembles of epistemic states (symbols) with corresponding classical observables, it is shown that such observables are complementary to each other with respect to particular partitions unless those partitions are generating. This explains why symbolic descriptions based on an ad hoc partition of an underlying phase space description should generally be expected to be incompatible. Related approaches with different background and different objectives are discussed
Electrically charged porous polytetrafluoroethylene (PTFE) films are often discussed as active layers for electromechanical transducers. Here, the electric charging behavior of open-porous PTFE films with different porosities is investigated. Optimized electric charging of porous PTFE films is determined by variation of charging parameters such as electric fields and charging times. Maximum surface potentials are depending on the porosity of the PTFE films. Suitable charging leads to high surface potentials observed on non-stretched or slightly stretched porous PTFE films. Further increase of charging fields yields decreasing values of the surface potential accompanied with an increase of conductivity.
We study possible interrelations between the 300-year record of the yearly sunspot numbers and the solar inertial motion (SIM) using the recently developed technique of synchronization analysis. Phase synchronization of the sunspot cycle and the SIM is found and statistically confirmed in three epochs (1734-1790, 1855-1875 and 1907-1960) of the whole period 1700-2000. These results give quantitative support to the hypothesis that there is a weak interaction between the solar activity and the SIM.
An approach for creating complex structures with embedded actuation in planar manufacturing steps is presented. Self-organization and energy minimization are central to this approach, illustrated with a model based on minimization of the hyperelastic free energy strain function of a stretched elastomer and the bending elastic energy of a plastic frame. A tulip-shaped gripper structure illustrates the technological potential of the approach. Advantages are simplicity of manufacture, complexity of final structures, and the ease with which any electroactive material can be exploited as means of actuation. (c) 2007 American Institute of Physics.
Energy-dispersive X-ray reflectivity and GID for real-time growth studies of pentacene thin films
(2007)
We use energy-dispersive X-ray reflectivity and grazing incidence diffraction (GID) to follow the growth of the crystalline organic semiconductor pentacene on silicon oxide in-situ and in real-time. The technique allows for monitoring Bragg reflections and measuring X-ray growth oscillations with a time resolution of 1 min in a wide q-range in reciprocal space extending over 0.25-0.80 angstrom(-1), i.e. sampling a large number of Fourier components simultaneously. A quantitative analysis of growth oscillations at several q-points yields the evolution of the surface roughness, showing a marked transition from layer-by-layer growth to strong roughening after four monolayers of pentacene have been deposited. (c) 2006 Elsevier B.V. All rights reserved.
Spectroscopic study of dielectric barrier discharges in cellular polypropylene ferroelectrets
(2007)
The transient light emission from the dielectric barrier discharges (DBDs) in cellular polypropylene ferroelectrets subjected to high electric poling fields was spectroscopically measured. The spectrum shows strong emission from the second positive system of molecular nitrogen, N-2(C (3)Pi(u))-> N-2(B (3)Pi(g)), and the first negative system of N-2(+), N-2(+)(B (2)Sigma(+)(u))-> N-2(+)(X (2)Sigma(+)(g)), consistent with a DBD in air. When a dc voltage is applied stepwise to the ferroelectret film, light emission starts above a threshold, coinciding with the threshold voltage in obtaining piezoelectricity. From selected vibronic band strength ratios, the electric field in the discharge was determined and found to agree with Townsend breakdown.
The dynamics and bifurcations of convective waves in rotating and buoyancy-driven spherical Rayleigh-Benard convection are investigated numerically. The solution branches that arise as rotating waves (RWs) are traced by means of path-following methods, by varying the Rayleigh number as a control parameter for different rotation rates. The dependence of the azimuthal drift frequency of the RWs on the Ekman and Rayleigh numbers is determined and discussed. The influence of the rotation rate on the generation and stability of secondary branches is demonstrated. Multistability is typical in the parameter range considered.
The strong adhesion of sub-micron sized particles to surfaces is a nuisance, both for removing contaminating colloids from surfaces and for conscious manipulation of particles to create and test novel micro/nano-scale assemblies. The obvious idea of using detergents to ease these processes suffers from a lack of control: the action of any conventional surface-modifying agent is immediate and global. With photosensitive azobenzene containing surfactants we overcome these limitations. Such photo-soaps contain optical switches (azobenzene molecules), which upon illumination with light of appropriate wavelength undergo reversible trans-cis photo-isomerization resulting in a subsequent change of the physico-chemical molecular properties. In this work we show that when a spatial gradient in the composition of trans- and cis- isomers is created near a solid-liquid interface, a substantial hydrodynamic flow can be initiated, the spatial extent of which can be set, e.g., by the shape of a laser spot. We propose the concept of light induced diffusioosmosis driving the flow, which can remove, gather or pattern a particle assembly at a solid-liquid interface. In other words, in addition to providing a soap we implement selectivity: particles are mobilized and moved at the time of illumination, and only across the illuminated area.
We study the adsorption–desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition—demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces—are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye–Hückel approximation is often not feasible and the nonlinear Poisson–Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson–Boltzmann equation is smaller than the Debye–Hückel result, such that the required critical surface charge density for polyelectrolyte adsorption σc increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical–chemical and biophysical systems.
We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the Néel temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost.
It is quite generally assumed that the overdamped Langevin equation provides a quantitative description of the dynamics of a classical Brownian particle in the long time limit. We establish and investigate a paradigm anomalous diffusion process governed by an underdamped Langevin equation with an explicit time dependence of the system temperature and thus the diffusion and damping coefficients. We show that for this underdamped scaled Brownian motion (UDSBM) the overdamped limit fails to describe the long time behaviour of the system and may practically even not exist at all for a certain range of the parameter values. Thus persistent inertial effects play a non-negligible role even at significantly long times. From this study a general questions on the applicability of the overdamped limit to describe the long time motion of an anomalously diffusing particle arises, with profound consequences for the relevance of overdamped anomalous diffusion models. We elucidate our results in view of analytical and simulations results for the anomalous diffusion of particles in free cooling granular gases.
We investigate the ensemble and time averaged mean squared displacements for particle diffusion in a simple model for disordered media by assuming that the local diffusivity is both fluctuating in time and has a deterministic average growth or decay in time. In this study we compare computer simulations of the stochastic Langevin equation for this random diffusion process with analytical results. We explore the regimes of normal Brownian motion as well as anomalous diffusion in the sub- and superdiffusive regimes. We also consider effects of the inertial term on the particle motion. The investigation of the resulting diffusion is performed for unconfined and confined motion.
What are the physical laws of the mutual interactions of objects bound to cell membranes, such as various membrane proteins or elongated virus particles? To rationalise this, we here investigate by extensive computer simulations mutual interactions of rod-like particles adsorbed on the surface of responsive elastic two-dimensional sheets. Specifically, we quantify sheet deformations as a response to adhesion of such filamentous particles. We demonstrate that tip-to-tip contacts of rods are favoured for relatively soft sheets, while side-by-side contacts are preferred for stiffer elastic substrates. These attractive orientation-dependent substrate-mediated interactions between the rod-like particles on responsive sheets can drive their aggregation and self-assembly. The optimal orientation of the membrane-bound rods is established via responding to the elastic energy profiles created around the particles. We unveil the phase diagramme of attractive–repulsive rod–rod interactions in the plane of their separation and mutual orientation. Applications of our results to other systems featuring membrane-associated particles are also discussed.
We report on rendering polyelectrolyte brushes photosensitive by loading them with azobenzene-containing cationic surfactants. Planar poly(methacrylic acid) (PMAA) brushes are synthesized using the “grafting from” free-radical polymerization scheme followed by exposure to a solution of photosensitive surfactants consisting of positively-charged head groups and hydrophobic tails into which azobenzene moieties are inserted. In this study the length of the hydrophobic methylene spacer connecting the azobenzene and the charged head group ranges from 4 to 10 CH2 groups. Under irradiation with UV light, the photo-isomerization of azobenzene integrated into a surfactant results in a change in size, geometry, dipole moment and free volume of the whole molecule. When the brush loaded with photosensitive surfactants is exposed to irradiation with UV interference patterns, the topography of the brush deforms following the distribution of the light intensity, exhibiting surface relief gratings (SRG). Since SRG formation is accompanied by a local rupturing of polymer chains in areas from which the polymer material is receding, most of the polymer material is removed from the surface during treatment with good solvent, leaving behind characteristic patterns of lines or dots. The azobenzene molecules still integrated within the polymer film can be removed by washing the brush with water. The remaining nano-structured brush can then be re-used for further functionalization. Although the opto-mechanically induced rupturing occurs for all surfactants, larger species do not penetrate deep enough into the brush such that after rupturing a leftover layer of polymer material remains on the substrate. This indicates that rupturing occurs predominantly in regions of high surfactant density.
Recombination of free charge is a key process limiting the performance of solar cells. For low mobility materials, such as organic semiconductors, the kinetics of non-geminate recombination (NGR) is strongly linked to the motion of charges. As these materials possess significant disorder, thermalization of photogenerated carriers in the inhomogeneously broadened density of state distribution is an unavoidable process. Despite its general importance, knowledge about the kinetics of NGR in complete organic solar cells is rather limited. We employ time delayed collection field (TDCF) experiments to study the recombination of photogenerated charge in the high-performance polymer:fullerene blend PCDTBT:PCBM. NGR in the bulk of this amorphous blend is shown to be highly dispersive, with a continuous reduction of the recombination coefficient throughout the entire time scale, until all charge carriers have either been extracted or recombined. Rapid, contact-mediated recombination is identified as an additional loss channel, which, if not properly taken into account, would erroneously suggest a pronounced field dependence of charge generation. These findings are in stark contrast to the results of TDCF experiments on photovoltaic devices made from ordered blends, such as P3HT:PCBM, where non-dispersive recombination was proven to dominate the charge carrier dynamics under application relevant conditions.
Compared to their inorganic counterparts, organic semiconductors suffer from relatively low charge carrier mobilities. Therefore, expressions derived for inorganic solar cells to correlate characteristic performance parameters to material properties are prone to fail when applied to organic devices. This is especially true for the classical Shockley-equation commonly used to describe current-voltage (JV)-curves, as it assumes a high electrical conductivity of the charge transporting material. Here, an analytical expression for the JV-curves of organic solar cells is derived based on a previously published analytical model. This expression, bearing a similar functional dependence as the Shockley-equation, delivers a new figure of merit α to express the balance between free charge recombination and extraction in low mobility photoactive materials. This figure of merit is shown to determine critical device parameters such as the apparent series resistance and the fill factor.
The gravitational field of a laser pulse of finite lifetime, is investigated in the framework of linearized gravity. Although the effects are very small, they may be of fundamental physical interest. It is shown that the gravitational field of a linearly polarized light pulse is modulated as the norm of the corresponding electric field strength, while no modulations arise for circular polarization. In general, the gravitational field is independent of the polarization direction. It is shown that all physical effects are confined to spherical shells expanding with the speed of light, and that these shells are imprints of the spacetime events representing emission and absorption of the pulse. Nearby test particles at rest are attracted towards the pulse trajectory by the gravitational field due to the emission of the pulse, and they are repelled from the pulse trajectory by the gravitational field due to its absorption. Examples are given for the size of the attractive effect. It is recovered that massless test particles do not experience any physical effect if they are co-propagating with the pulse, and that the acceleration of massless test particles counter-propagating with respect to the pulse is four times stronger than for massive particles
at rest. The similarities between the gravitational effect of a laser pulse and Newtonian gravity in two dimensions are pointed out. The spacetime curvature close to the pulse is compared to that induced by gravitational waves from astronomical sources.