Ultrafast Electron Diffraction with Spatiotemporal Resolution of Atomic Motion

Ultrafast electron diffraction （UED） is a rapidly advancing technique capable of recording the atomic-detail structural dynamics in real time. We report the establishment of the first UED system in China. Employing this UED apparatus, both the coherent and the concurrent thermal lattice motions in an aluminium thin-film, trigged by ultrafast laser heating, have been observed. These results demonstrate its ability to directly measure a sub-milli-angstrom lattice spacing change on a sub-picosecond time scale.     

Selective recognition of ovalbumin using a molecularly imprinted polymer

Micro-contact imprinting has been used to form thin-film molecular imprints of ovalbumin (OVA) in polymers supported on glass slides. Thermocalorimetric data was used to optimise the choice of functional monomer and cross-linker to maximise selectivity and minimise non-specific recognition.A polymer comprising polyethyleneglycol 400 dimethacrylate (95 vol.%) and methacrylic acid (5 vol.%) showed both maximum recognition for OVA when made as a molecularly imprinted polymer (MIP), and minimal recognition when made as a non-imprinted, i.e. control polymer. OVA rebinding to the molecularly imprinted polymer, from a buffered 2 µM OVA solution, was 1.55 × 10^{− 11} mol cm^{− 2}, while the control polymer showed 10-fold less re-binding, i.e. 0.154 × 10^{− 11} mol cm^{− 2}.Experiments in which human serum albumin (HSA), conalbumin, ovomucoid or lysozyme, were re-bound to the polymers, either as single proteins or in competition with OVA, showed them to have low affinity for the polymer formulation used. Of the competing proteins examined, in non-competitive binding experiments, HSA showed the greatest affinity 0.45 × 10^{− 11} mol cm^{− 2} for the OVA imprinted polymer. In two protein competition experiments, i.e. with OVA and a competing protein present at equal concentrations (2 µM), OVA binding to the OVA imprinted polymer was in all cases significantly greater than that of the competitor.     

Side chain mediated electronic contact between a tetrahydro-4H-thiopyran-4-ylidene-appended polythiophene and CdTe quantum dots

The properties of a mixed CdTe quantum dot/tetrahydro-4H-thiopyran-4-ylidene-functionalized polythiophene system are reported. This system was prepared by exposing trioctylphosphine (TOP)-capped CdTe quantum dots to the polythiophene in solution. Strong fluorescence emission quenching and shortening of the fluorescence emission lifetimes of both the polythiophene and the quantum dots occur when they are mixed, indicating the occurrence of photoinduced charge separation. Photoinduced absorption spectroscopy reveals a considerable decrease in the population of the polythiophene triplet excited state in the mixed system. These results demonstrate that between the quantum dots and the polythiophene there is both physical and electronic contact, which is mediated by the tetrahydro-4H-thiopyran-4-ylidene side chains.     

Effect of tones on vocal attack time in Cantonese speakers

Vocal attack time (VAT) is the time lag between the growth of the sound pressure signal and the development of physical contact of vocal folds at vocal initiation. It can be derived by a cross-correlation of short-time amplitude changes occurring in the sound pressure and electroglottographic (EGG) signals. Cantonese is a tone language in which tone determines the lexical meaning of the syllable. Such linguistic function of tone has implications for the physiology of tone production. The aim of the present study was to investigate the possible effects of Cantonese tones on VAT. Sound pressure and EGG signals were simultaneously recorded from 59 native Cantonese speakers (31 females and 28 males). The subjects were asked to read aloud 12 disyllabic words comprising homophone pairs of the six Cantonese lexical tones. Results revealed a gender difference in VAT values, with the mean VAT significantly smaller in females than in males. There was also a significant difference in VAT values between the two tone categories, with the mean VAT values of the three level tones (tone 1, 3, and 6) significantly smaller than those of the three contour tones (tone 2, 4, and 5). The findings support the notion that norms and interpretations based on nontone European languages may not be directly applied to tone languages.     

Formation of N719 dye multilayers on dye sensitized solar cell photoelectrode surfaces investigated by direct determination of element concentration depth profiles

The structure of the dye layer adsorbed on the titania substrate in a dye-sensitized solar cell is of fundamental importance for the function of the cell, since it strongly influences the injection of photoelectrons from the excited dye molecules into the titania substrate. The adsorption isotherms of the N719 ruthenium-based dye were determined both with a direct method using the depth profiling technique neutral impact collision ion scattering spectroscopy (NICISS) and with the standard indirect solution depletion method. It is found that the dye layer adsorbed on the titania surface is laterally inhomogeneous in thickness and there is a growth mechanism already from low coverage levels involving a combination of monolayers and multilayers. It is also found that the amount of N719 adsorbed on the substrate depends on the titania structure. The present results show that dye molecules in dye-sensitized solar cells are not necessarily, as presumed, adsorbed as a self-assembled monolayer on the substrate.     

Chutes and Ladders in Markov Chains

We investigate how the stationary distribution of a Markov chain changes when transitions from a single state are modified. In particular, adding a single directed edge to nearest neighbor random walk on a finite discrete torus in dimensions one, two, or three changes the stationary distribution linearly, logarithmically, or only locally. Related results are derived for birth and death chains approximating Bessel diffusions and for random walk on the Sierpinski gasket.     

Combined Photoredox and Carbene Catalysis for the Synthesis of Ketones from Carboxylic Acids**

As a key element in the construction of complex organic scaffolds, the formation of C−C bonds remains a challenge in the field of synthetic organic chemistry. Recent advancements in single-electron chemistry have enabled new methods for the formation of various C−C bonds. Disclosed herein is the development of a novel single-electron reduction of acyl azoliums for the formation of ketones from carboxylic acids. Facile construction of the acyl azolium in situ followed by a radical–radical coupling was made possible merging N-heterocyclic carbene (NHC) and photoredox catalysis. The utility of this protocol in synthesis was showcased in the late-stage functionalization of a variety of pharmaceutical compounds. Preliminary investigations using chiral NHCs demonstrate that enantioselectivity can be achieved, showcasing the advantages of this protocol over alternative methodologies.     

‘Praying Mantis’ diffuse reflectance accessory for UV-Vis-NIR spectroscopy

Conclusion The characteristics of the PM accessory allow reflecting measurements on a new variety of samples such as fruits, vegetables, tissue cultures, fermentation broths or reagent-impregnated dip sticks currently being developed for clinical laboratories.     

On weighted heights of random trees

Consider the family treeT of a branching process starting from a single progenitor and conditioned to havev=v(T) edges (total progeny). To each edge <e> we associate a weightW(e). The weights are i.i.d. random variables and independent ofT. The weighted height of a self-avoiding path inT starting at the root is the sum of the weights associated with the path. We are interested in the asymptotic distribution of the maximum weighted path height in the limit asv=n. Depending on the tail of the weight distribution, we obtain the limit in three cases. In particular ify ² P(W(e)> y)0, then the limit distribution depends strongly on the tree and, in fact, is the distribution of the maximum of a Brownian excursion. If the tail of the weight distribution is regularly varying with exponent 0<2, then the weight swamps the tree and the answer is the asymptotic distribution of the maximum edge weight in the tree. There is a borderline case, namely,P(W(e)> y)cy ^–2 asy, in which the limit distribution exists but involves both the tree and the weights in a more complicated way.