Resonance tongues in a system of globally coupled FitzHugh-Nagumo oscillators with time-periodic coupling strength

We investigate the dynamics of a population of globally coupled FitzHugh-Nagumo oscillators with a time-periodic coupling strength. While for synchronizing global coupling, the in-phase state is always stable, the oscillators split into several cluster states for desynchronizing global coupling, most commonly in two, irrespective of the coupling strength. This confines the ability of the system to form n:m locked states considerably. The prevalence of two and four cluster states leads to large 2:1 and 4:1 subharmonic resonance regions, while at low coupling strength for a harmonic 1:1 or a superharmonic 1:m time-periodic coupling coefficient, any resonances are absent and the system exhibits nonresonant phase drifting cluster states. Furthermore, in the unforced, globally coupled system the frequency of the oscillators in a cluster state is in general lower than that of the uncoupled oscillator and strongly depends on the coupling strength. Periodic variation of the coupling strength at twice the natural frequency causes each oscillator to keep oscillating with its autonomous oscillation period.     

Entropy and Free Energy of a Mobile Loop Based on the Crystal Structures of the Free and Bound Proteins

A mobile loop changes its conformation from "open" (free enzyme) to "closed" upon ligand binding. The difference in the Helmholtz free energy, ΔF(loop) between these states sheds light on the mechanism of binding. With our "hypothetical scanning molecular dynamics" (HSMD-TI) method ΔF(loop) = F(free) - F(bound) where F(free) and F(bound) are calculated from two MD samples of the free and bound loop states; the contribution of water is obtained by a thermodynamic integration (TI) procedure. In previous work the free and bound loop structures were both attached to the same "template" which was "cut" from the crystal structure of the free protein. Our results for loop 287-290 of AcetylCholineEsterase agree with the experiment, ΔF(loop)~ -4 kcal/mol if the density of the TIP3P water molecules capping the loop is close to that of bulk water, i.e., N(water) = 140 - 180 waters in a sphere of a 18 ? radius. Here we calculate ΔF(loop) for the more realistic case, where two templates are "cut" from the crystal structures, 2dfp.pdb (bound) and 2ace.pdb (free), where N(water) = 40 - 160; this requires adding a computationally more demanding (second) TI procedure. While the results for N(water) ≤ 140 are computationally sound, ΔF(loop) is always positive (18 ± 2 kcal/mol for N(water) = 140). These (disagreeing) results are attributed to the large average B-factor, 41.6 of 2dfp (23.4 ?(2) for 2ace). While this conformational uncertainty is an inherent difficulty, the (unstable) results for N(water) = 160 suggest that it might be alleviated by applying different (initial) structural optimizations to each template.     

Ionization mechanism in gel permeation chromatography mass spectrometry (GPC-MS) with atmospheric pressure chemical ionization (APCI) interface

The ionization mechanism in gel permeation chromatography (GPC) coupled with mass spectrometry (MS) using an atmospheric pressure chemical ionization (APCI) interface is explained when chloroform is used as GPC solvent. The even electron anions [CHCl₃+Cl]^? generated by thermal electrons in negative APCI mode are responsible for further ionization of the solute compounds as [M?+?Cl]^? adducts. In positive APCI mode, the contaminants in chloroform generate a relatively high background noise. These cations can be suppressed by adding 10% of tetrahydrofuran (THF). Supporting the described mechanism are key experiments done in the absence of solvent, in GPC solvents and using a mixture of anionic polystyrene (PS) standards from dimer up to 12,000?g/mol, covering the molecular masses of great interest in studies related to Registration, Evaluation, Authorization, and Restriction of Chemicals (REACH) and Food and Drug Administration (FDA). Advantages of suppressing the oligomer signals for polymer additive analyses were presented using Irgafos^® 168.     

A Z‐Scheme‐Inspired Photobioelectrochemical H2O/O2 Cell with a 1 V Open‐Circuit Voltage Combining Photosystem II and PbS Quantum Dots

A biohybrid photobioanode mimicking the Z‐scheme has been developed by functional integration of photosystem II (PSII) and PbS quantum dots (QDs) within an inverse opal TiO₂ architecture giving rise to a rather negative water oxidation potential of about ?0.55 V vs. Ag/AgCl, 1 m KCl at neutral pH. The electrical linkage between both light‐sensitive entities has been established through an Os‐complex‐modified redox polymer (P_Os), which allows the formation of a multi‐step electron‐transfer chain under illumination starting with the photo‐activated water oxidation at PSII followed by an electron transfer from PSII through P_Os to the photo‐excited QDs and finally to the TiO₂ electrode. The photobioanode was coupled to a novel, transparent, inverse‐opal ATO cathode modified with an O₂‐reducing bilirubin oxidase for the construction of a H₂O/O₂ photobioelectrochemical cell reaching a high open‐circuit voltage of about 1 V under illumination.     

Toward sustainable energy: photocatalysis of Cr-doped TiO<Subscript>2</Subscript>: 2. effect of defect disorder

The present chain of five papers considers the concept of solar-to-chemical energy conversion using TiO₂-based semiconductors. The series reports the effect of chromium on the key performance-related properties of polycrystalline TiO₂ (rutile), including electronic structure, photocatalytic activity, intrinsic defect disorder, electrochemical coupling and surface versus bulk properties. In this work, we show that the effect of chromium on photocatalytic performance of TiO₂ depends on its elemental content and the related defect disorder that is determined by oxygen activity in the oxide lattice. At high oxygen activity, chromium leads to enhanced photocatalytic performance only for dilute solid solutions (up to 0.04–0.043 at.% Cr). Higher chromium content results in a decrease of photocatalytic activity below that for pure TiO₂, despite the observed substantial decrease of the band gap. The photocatalytic performance of Cr-doped TiO₂ annealed in reducing conditions is low within the entire studied range of compositions. The obtained results led to derivation of a theoretical model representing the mechanism of the light-induced reactivity of TiO₂ with water and the related charge transfer. The photocatalytic performance is considered in terms of a competitive effect of several key performance-related properties. The performance is predominantly influenced by the concentration of titanium vacancies acting as reactive surface sites related to anodic charge transfer.

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International perspective on nanotechnology papers,patents, and NSF awards (2000–2016)

This paper presents the development of nanotechnology between 2000 and 2016 as reflected in the Web of Science papers, United States Patent and Trademark Office (USPTO), World International Property Organization (WIPO) patents, and National Science Foundation (NSF) awards, with a special reference to the United States (US), European Union (EU27), P.R. China, Japan, and South Korea. The field of nanotechnology is branching out into novel scientific and technology platforms, and it is increasingly difficult to separate foundational nanoscale components from divergent application areas. The average global growth rate has been sustained at about 15% for both papers and patents in the selected interval. The growth rates among regions are non-uniform. P.R. China and South Korea have increased faster in both the numbers and quality of their scientific publications, and currently P.R. China has the largest volume of nanotechnology publications and South Korea the most publications per capita in the field of nanotechnology. The US, EU27, and Japan are maintaining leadership in the upstream, better cited, conceptual components of nanotechnology research and development.     

Quantum Transport in Presence of Bound States – Noise Power

The impact of bound states in Landauer‐Büttiker scattering approach to non‐equilibrium quantum transport is investigated. We show that the noise power at frequency ν is sensitive to all bound states with energies ω_b satisfying . We derive the exact expression of the bound state contribution and compare it to the one produced by the scattering states alone. The theoretical and experimental consequences of this result are discussed.     

Quantitative imaging of single, unstained viruses with coherent x rays

We report the recording and reconstruction of x-ray diffraction patterns from single, unstained viruses, for the first time. By separating the diffraction pattern of the virus particles from that of their surroundings, we performed quantitative and high-contrast imaging of a single virion. The structure of the viral capsid inside a virion was visualized. This work opens the door for quantitative x-ray imaging of a broad range of specimens from protein machineries and viruses to cellular organelles. Moreover, our experiment is directly transferable to the use of x-ray free electron lasers, and represents an experimental milestone towards the x-ray imaging of large protein complexes.     

Infinite randomness fixed point of the superconductor-metal quantum phase transition

We examine the influence of quenched disorder on the superconductor-metal transition, as described by a theory of overdamped Cooper pairs which repel each other. The self-consistent pairing eigenmodes of a quasi-one-dimensional wire are determined numerically. Our results support the recent proposal by Hoyos et al. [Phys. Rev. Lett. 99, 230601 (2007)10.1103/PhysRevLett.99.230601] that the transition is characterized by the same strong-disorder fixed point describing the onset of ferromagnetism in the random quantum Ising chain in a transverse field.