Cross‐Coupling Reactions between Stable Carbenes

By utilizing stable carbenes with low‐lying LUMOs, coupling with the stable nucleophilic diaminocyclopropenylidene was achieved. This reaction resulted in the formation of two new and rare examples of a bent allene as well as the isolation of the first carbene–carbene heterodimer.     

Pure insulin nanoparticle agglomerates for pulmonary delivery

Diabetes is a set of diseases characterized by defects in insulin utilization, either through autoimmune destruction of insulin-producing cells (Type I) or insulin resistance (Type II). Treatment options can include regular injections of insulin, which can be painful and inconvenient, often leading to low patient compliance. To overcome this problem, novel formulations of insulin are being investigated, such as inhaled aerosols. Sufficient deposition of powder in the peripheral lung to maximize systemic absorption requires precise control over particle size and density, with particles between 1 and 5 microm in aerodynamic diameter being within the respirable range. Insulin nanoparticles were produced by titrating insulin dissolved at low pH up to the pI of the native protein, and were then further processed into microparticles using solvent displacement. Particle size, crystallinity, dissolution properties, structural stability, and bulk powder density were characterized. We have demonstrated that pure drug insulin microparticles can be produced from nanosuspensions with minimal processing steps without excipients, and with suitable properties for deposition in the peripheral lung.     

Scaling laws in NMR scattering via dipolar fields

Breaking translational symmetry in magnetostatics imparts a scale dependence that is commonly investigated in physics (W. Warren et al., 1993, Science 262, 2005-2008). An interesting and important example arises in nuclear magnetic resonance studies involving the dipolar mean field of adjacent nuclear spins where the scattering (transfer of spatial spin gratings) via intermolecular macroscopic fields carries a signature of the local spatial distribution of the spin density. For arbitrary geometry, the inverse problem of extracting this spin distribution from experiments is intractable. Here we point out a simple, universal crossover in the scaling behavior at the sample's characteristic length scale, xi, of the species fluctuations in the sample along the measurement direction. This behavior is observed experimentally in an oil-water emulsion, an important representation of complex, heterogeneous, soft matter.     

Reversible surface electronic traps in PbS quantum dot solids induced by an order-disorder phase transition in capping molecules

The electronic properties of semiconductor quantum dots (QDs) are critically dependent on the nature of the ligand molecules on their surfaces. Here we show the reversible formation of surface electronic trap states in the model system of solid thin films of PbS QDs capped with thiol molecules. As the temperature was increased from cryogenic to room temperature, we discovered a phase transition in the fluorescence spectra from excitonic emission to trap emission. The critical temperature (T(c)) of the phase transition scales with molecular length and in each case is close to the bulk melting temperature of the capping molecules. We conclude that an order-disorder transition in the molecular monolayer above T(c) introduces surface mobility and the formation of a disordered atomic lead layer at the QD/capping molecule interface, leading to electronic trap formation.     

Asymptotic analysis of collision-induced timing shifts in return-to-zero quasi-linear systems with predispersion and postdispersion compensation

An asymptotic method for calculating the collision-induced frequency and timing shifts for quasi-linear pulses in return-to-zero, wavelength-division multiplexed systems with predispersion and postdispersion compensation is developed. Predictions of the asymptotic theory agree well with quadrature and direct numerical simulations. Using this theory, computational savings of many orders of magnitude can be realized over direct numerical simulations.     

Single spin measurement using cellular automata techniques

We analyze a conceptual approach to single-spin measurement. The method uses techniques from the theory of quantum cellular automata to correlate a large number of ancillary spins to the one to be measured. It has the distinct advantage of being efficient: under ideal conditions, it requires the application of only O((3)square root N)) steps (each requiring a constant number of rf pulses) to create a system of N correlated spins. Numerical simulations suggest that it is also, to a certain extent, robust against pulse errors, and imperfect initial polarization of the ancilla spin system.     

ChemInform Abstract: An ab initio Investigation of Bismuth Hydration.

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