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Diffusion of finite-size particles in two-dimensional channels with random wall configurations
(2014)
Diffusion of chemicals or tracer molecules through complex systems containing irregularly shaped channels is important in many applications. Most theoretical studies based on the famed Fick–Jacobs equation focus on the idealised case of infinitely small particles and reflecting boundaries. In this study we use numerical simulations to consider the transport of finite-size particles through asymmetrical two-dimensional channels. Additionally, we examine transient binding of the molecules to the channel walls by applying sticky boundary conditions. We consider an ensemble of particles diffusing in independent channels, which are characterised by common structural parameters. We compare our results for the long-time effective diffusion coefficient with a recent theoretical formula obtained by Dagdug and Pineda [J. Chem. Phys., 2012, 137, 024107].
We report the first-ever discovery of a Wolf-Rayet (WR) star in the Large Magellanic Cloud via detection of a circular shell with the Spitzer Space Telescope. Follow-up observations with Gemini-South resolved the central star of the shell into two components separated from each other by a parts per thousand 2 arcsec (or a parts per thousand 0.5 pc in projection). One of these components turns out to be a WN3 star with H and He lines both in emission and absorption (we named it BAT99 3a using the numbering system based on extending the Breysacher et al. catalogue). Spectroscopy of the second component showed that it is a B0 V star. Subsequent spectroscopic observations of BAT99 3a with the du Pont 2.5-m telescope and the Southern African Large Telescope revealed that it is a close, eccentric binary system, and that the absorption lines are associated with an O companion star. We analysed the spectrum of the binary system using the non-LTE Potsdam WR (powr) code, confirming that the WR component is a very hot (a parts per thousand 90 kK) WN star. For this star, we derived a luminosity of log L/ L-aS (TM) = 5.45 and a mass-loss rate of 10(- 5.8) M-aS (TM) yr(- 1), and found that the stellar wind composition is dominated by helium with 20 per cent of hydrogen. Spectroscopy of the shell revealed an He iii region centred on BAT99 3a and having the same angular radius (a parts per thousand 15 arcsec) as the shell. We thereby add a new example to a rare class of high-excitation nebulae photoionized by WR stars. Analysis of the nebular spectrum showed that the shell is composed of unprocessed material, implying that the shell was swept-up from the local interstellar medium. We discuss the physical relationship between the newly identified massive stars and their possible membership of a previously unrecognized star cluster.
This Letter reports the discovery of a remarkably hard spectrum source, HESS J1641-463, by the High Energy Stereoscopic System (H.E.S.S.) in the very high energy (VHE) domain. HESS J1641-463 remained unnoticed by the usual analysis techniques due to confusion with the bright nearby source HESS J1640-465. It emerged at a significance level of 8.5 standard deviations after restricting the analysis to events with energies above 4 TeV. It shows a moderate flux level of phi(E > 1TeV) = (3.64 +/- 0.44(stat)+/- 0.73(sys)) x 10(-13) cm(-2) s(-1), corresponding to 1.8% of the Crab Nebula flux above the same energy, and a hard spectrum with a photon index of Gamma = 2.07 +/- 0.11(stat)+/- 0.20(sys). It is a point-like source, although an extension up to a Gaussian width of sigma = 3 arcmin cannot be discounted due to uncertainties in the H.E.S.S. point-spread function. The VHE gamma-ray flux of HESS J1641-463 is found to be constant over the observed period when checking time binnings from the year-by-year to the 28 minute exposure timescales. HESS J1641-463 is positionally coincident with the radio supernova remnant SNR G338.5+0.1. No X-ray candidate stands out as a clear association; however, Chandra and XMM-Newton data reveal some potential weak counterparts. Various VHE gamma-ray production scenarios are discussed. If the emission from HESS J1641-463 is produced by cosmic ray protons colliding with the ambient gas, then their spectrum must extend close to 1 PeV. This object may represent a source population contributing significantly to the galactic cosmic ray flux around the knee.
X-ray emission from stars much more massive than the Sun was discovered only 35 years ago. Such stars drive fast stellar winds where shocks can develop, and it is commonly assumed that the X-rays emerge from the shock-heated plasma. Many massive stars additionally pulsate. However, hitherto it was neither theoretically predicted nor observed that these pulsations would affect their X-ray emission. All X-ray pulsars known so far are associated with degenerate objects, either neutron stars or white dwarfs. Here we report the discovery of pulsating X-rays from a non-degenerate object, the massive B-type star xi(1) CMa. This star is a variable of beta Cep-type and has a strong magnetic field. Our observations with the X-ray Multi-Mirror (XMM-Newton) telescope reveal X-ray pulsations with the same period as the fundamental stellar oscillations. This discovery challenges our understanding of stellar winds from massive stars, their X-ray emission and their magnetism.
We investigate the time-dependent Casimir-Polder potential of a polarizable two-level atom placed near a surface of arbitrary material, after a sudden change in the parameters of the system. Different initial conditions are taken into account. For an initially bare ground-state atom, the time-dependent Casimir-Polder energy reveals how the atom is "being dressed" by virtual, matter-assisted photons. We also study the transient behavior of the Casimir-Polder interaction between the atom and the surface starting from a partially dressed state, after an externally induced change in the atomic level structure or transition dipoles. The Heisenberg equations are solved through an iterative technique for both atomic and field operators in the medium-assisted electromagnetic field quantization scheme. We analyze, in particular, how the time evolution of the interaction energy depends on the optical properties of the surface, in particular on the dispersion relation of surface plasmon polaritons. The physical significance and the limits of validity of the obtained results are discussed in detail.
In resonant inelastic soft x-ray scattering (RIXS) from molecular and liquid systems, the interplay of ground state structural and core-excited state dynamical contributions leads to complex spectral shapes that partially allow for ambiguous interpretations. In this work, we dissect these contributions in oxygen K-edge RIXS from liquid alcohols. We use the scattering into the electronic ground state as an accurate measure of nuclear dynamics in the intermediate core-excited state of the RIXS process. We determine the characteristic time in the core-excited state until nuclear dynamics give a measurable contribution to the RIXS spectral profiles to tau(dyn) = 1.2 +/- 0.8 fs. By detuning the excitation energy below the absorption resonance we reduce the effective scattering time below sdyn, and hence suppress these dynamical contributions to a minimum. From the corresponding RIXS spectra of liquid methanol, we retrieve the "dynamic-free" density of states and find that it is described solely by the electronic states of the free methanol molecule. From this and from the comparison of normal and deuterated methanol, we conclude that the split peak structure found in the lone-pair emission region at non-resonant excitation originates from dynamics in the O-H bond in the core-excited state. We find no evidence that this split peak feature is a signature of distinct ground state structural complexes in liquid methanol. However, we demonstrate how changes in the hydrogen bond coordination within the series of linear alcohols from methanol to hexanol affect the split peak structure in the liquid alcohols. (C) 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.
The contraction/swelling transition of anionic PNIPAM-co-AAA particles can be manipulated by light using interactions with cationic azobenzene-containing surfactant. In this study the influence of pH-buffers and their concentrations, the charge density (AAA content) in microgel particles as well as the spacer length of the surfactant on the complex formation between the microgel and surfactant is investigated. It is shown that the presence of pH buffer can lead to complete blocking of the interactions in such complexes and the resulting microgel contraction/swelling response. There is a clear competition between the buffer ions and the surfactant molecules interacting with microgel particles. When working in pure water solutions with fixed concentration (charge density) of microgel, the contraction/swelling of the particles is controlled only by relative concentration (charge ratio) of the surfactant and AAA groups of the microgel. Furthermore, the particle contraction is more efficient for shorter spacer length of the surfactant. The onset point of the contraction process is not affected by the surfactant hydrophobicity. This work provides new insight into the interaction between microgel particles and photo-sensitive surfactants, which offers high potential in new sensor systems. (C) 2014 Elsevier Ltd. All rights reserved.
The charge generation and recombination processes following photo-excitation of a low-bandgap polymer:perylene diimide photovoltaic blend are investigated by transient absorption pump-probe spectroscopy covering a dynamic range from femto-to microseconds to get insight into the efficiency-limiting photophysical processes. The several tens of picoseconds, and its efficiency is only half of that in a polymer:fullerene photoinduced electron transfer from the polymer to the perylene acceptor takes up to blend. This reduces the short-circuit current. Time-delayed collection field experiments reveal that the subsequent charge separation is strongly field-dependent, limiting the fill factor and lowering the short-circuit current in polymer:PDI devices. Upon excitation of the acceptor in the low-bandgap polymer blend, the PDI exciton undergoes charge transfer on a time scale of several tens of picoseconds. However, a significant fraction of the charges generated at the interface are quickly lost because of fast geminate recombination. This reduces the short-circuit current even further, leading to a scenario in which only around 2596 of the initial photoexcitations generate free charges that can potentially contribute to the photocurrent. In summary, the key photophysical limitations of perylene diimide as an acceptor in low-bandgap polymer blends appear at the interface between the materials, with the kinetics of both charge generation and separation inhibited as compared to that of fullerenes.
carriers on illumination. Efficient organic solar cells require a high yield for this process, combined with a minimum of energy losses. Here, we investigate the role of the lowest energy emissive interfacial charge-transfer state (CT1) in the charge generation process. We measure the quantum yield and the electric field dependence of charge generation on excitation of the charge-transfer (CT) state manifold viaweakly allowed, low-energy optical transitions. For a wide range of photovoltaic devices based on polymer: fullerene, small-molecule:C-60 and polymer: polymer blends, our study reveals that the internal quantum efficiency (IQE) is essentially independent of whether or not D, A or CT states with an energy higher than that of CT1 are excited. The best materials systems show an IQE higher than 90% without the need for excess electronic or vibrational energy.