School of Chemistry - Research Publications
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ItemLight losses from scattering in luminescent solar concentrator waveguides(OPTICAL SOC AMER, 2017-04-01)The reductions in the transmission of emission originating from a fluorophore dissolved in a polymer matrix due to light scattering were compared in two forms of planar waveguides used as luminescent solar concentrators: a thin film of poly(methylmethacrylate) (PMMA) spin-coated on a glass plate and a solid PMMA plate of the same dimensions. The losses attributable to light scattering encountered in the waveguide consisting of the thin film of polymer coated on a glass plate were not detectable within experimental uncertainty, whereas the losses in the solid polymer plate were significant. The losses in the solid plate are interpreted as arising from light-scattering centers comprising minute bubbles of vapor/gas, incomplete polymerization or water clusters that are introduced during or after the thermally induced polymerization process.
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ItemSpatially Resolved Photophysical Dynamics in Perovskite Microplates Fabricated Using an Antisolvent Treatment(American Chemical Society, 2017-11-30)Perovskite microplates have important implications in the fields of functional electronics and optoelectronics. We report a facile strategy, antisolvent treatment for the growth of perovskite microplates. The morphology and crystalline quality of the microplates could be controlled by the amount of the chlorobenzene antisolvent used. An appropriate amount of antisolvent facilitates the formation of high-quality perovskite microplates with no residual precursor remaining. Spatially and temporally resolved fluorescence measurements demonstrate the heterogeneity of defect-state density and recombination processes in various perovskite microplate regions. The body center shows higher defect state density when compared with that at the edge or the corner of the microplate. Excessive antisolvent degrades the microplates into smaller particles. The results of this study reveal the factors that influence the crystallization process and photophysical dynamics of perovskite microplates.
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ItemPoly(3-hexylthiophene) coated graphene oxide for improved performance of bulk heterojunction polymer solar cells(Elsevier, 2017-05-01)An effective method for preparing poly(3-hexylthiophene) (P3HT) coated graphene oxide (GO), (P-GO), based on an ethanol mediated mixing and solvent evaporation method is described. P-GO exhibits good dispersibility in the non-polar solvent o-dichlorobenzene (DCB) allowing the preparation of polymer blend composites. P-GO was doped into P3HT: PCBM blends by solution mixing and shown to facilitate phase separation of P3HT and PCBM in P3HT: PCBM blend films to achieve a more optimum morphology for polymer photovoltaic cells. Bulk heterojunction P3HT: PCBM solar cells exhibit ∼18% power conversion efficiency enhancement in the presence of P-GO.
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ItemElectronic Structure Engineering in ZnSe/CdS Type-II Nanoparticles by Interface Alloying(American Chemical Society, 2014-06-19)We report the synthesis and characterization of type-II ZnSe/CdS semiconductor nanocrystals that exhibit strong charge separation, high photoluminescence quantum yields, low optical gain thresholds, and alloyed core–shell interfaces. Shell growth rates and the degree of alloying both depend strongly on the shelling temperature. The core–shell NCs exhibit band edge PL with emission wavelengths spanning the blue to orange region of the electromagnetic spectrum (380–562 nm). Fluorescence quantum yields up to 75% can be obtained by deposition of an additional ZnS layer. Transient absorption spectroscopy reveals that the population of the first two exciton states (1Se–1Sh, 1Se–2Sh) in the type-II structures can be controlled by alloying. Increased alloying leads to a greater population of the 2S hole state exciton.
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ItemNanoscale magnetometry through quantum control of nitrogen-vacancy centres in rotationally diffusing nanodiamonds(IOP Publishing, 2013)The confluence of quantum physics and biology is driving a new generation of quantum-based sensing and imaging technology capable of harnessing the power of quantum effects to provide tools to understand the fundamental processes of life. One of the most promising systems in this area is the nitrogen–vacancy centre in diamond—a natural spin qubit which remarkably has all the right attributes for nanoscale sensing in ambient biological conditions. Typically the nitrogen–vacancy qubits are fixed in tightly controlled/isolated experimental conditions. In this work quantum control principles of nitrogen–vacancy magnetometry are developed for a randomly diffusing diamond nanocrystal. We find that the accumulation of geometric phases, due to the rotation of the nanodiamond plays a crucial role in the application of a diffusing nanodiamond as a bio-label and magnetometer. Specifically, we show that a freely diffusing nanodiamond can offer real-time information about local magnetic fields and its own rotational behaviour, beyond continuous optically detected magnetic resonance monitoring, in parallel with operation as a fluorescent biomarker.
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ItemDFT Studies on the Stereoselectivity of α-Silyloxy Diazoalkane Cycloadditions.(MDPI AG, 2015-12-02)The intramolecular [3+2] cycloaddition (32CA) of alkene-tethered α-silyloxydiazoalkanes provides variable stereoselectivity in generating bicyclic pyrazolines where the silyloxy group is either syn or anti to the newly formed pyrazoline ring. To elucidate the origin of the stereoselectivity, density functional theory (DFT) calculations were carried out for the energy of each transition state structure (TSs) and product. Steric effects were identified as the major determining factors in the diastereoselectivity of the 32CA reaction with regards to substrate structure (cyclic or acyclic α-silyloxydiazoalkanes).
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ItemA monophasic extraction strategy for the simultaneous lipidome analysis of polar and nonpolar retina lipids(ELSEVIER, 2014-08)Lipid extraction using a monophasic chloroform/methanol/water mixture, coupled with functional group selective derivatization and direct infusion nano-ESI-high-resolution/accurate MS, is shown to facilitate the simultaneous analysis of both highly polar and nonpolar lipids from a single retina lipid extract, including low abundance highly polar ganglioside lipids, nonpolar sphingolipids, and abundant glycerophospholipids. Quantitative comparison showed that the monophasic lipid extraction method yielded similar lipid distributions to those obtained from established "gold standard" biphasic lipid extraction methods known to enrich for either highly polar gangliosides or nonpolar lipids, respectively, with only modest relative ion suppression effects. This improved lipid extraction and analysis strategy therefore enables detailed lipidome analyses of lipid species across a broad range of polarities and abundances, from minimal amounts of biological samples and without need for multiple lipid class-specific extractions or chromatographic separation prior to analysis.
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Itemn-3 PUFAs enhance the frequency of murine B-cell subsets and restore the impairment of antibody production to a T-independent antigen in obesity(ELSEVIER, 2013-11)The role of n-3 polyunsaturated fatty acids (PUFA) on in vivo B-cell immunity is unknown. We first investigated how n-3 PUFAs impacted in vivo B-cell phenotypes and antibody production in the absence and presence of antigen compared with a control diet. Lean mice consuming n-3 PUFAs for 4 weeks displayed increased percentage and frequency of splenic transitional 1 B cells. Upon stimulation with trinitrophenylated-lipopolysaccharide, n-3 PUFAs increased the number of splenic transitional 1/2, follicular, premarginal, and marginal zone B cells. n-3 PUFAs also increased surface, but not circulating, IgM. We next tested the effects of n-3 PUFAs in a model of obesity that is associated with suppressed humoral immunity. An obesogenic diet after ten weeks of feeding, relative to a lean control, had no effect on the frequency of B cells but lowered circulating IgM upon antigen stimulation. Administration of n-3 PUFAs to lean and obese mice increased the percentage and/or frequency of transitional 1 and marginal zone B cells. Furthermore, n-3 PUFAs in lean and obese mice increased circulating IgM relative to controls. Altogether, the data show n-3 PUFAs enhance B cell-mediated immunity in vivo, which has implications for immunocompromised populations, such as the obese.
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ItemTuning the properties of pH responsive nanoparticles to control cellular interactions in vitro and ex vivo(ROYAL SOC CHEMISTRY, 2016-01-01)Engineering the properties of nanoparticles to limit non-specific cellular interactions is critical for developing effective drug delivery systems. Differences between interactions with cultured cells and human blood highlights the need for appropriate assays
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ItemIntegrated activities of two alternative sigma factors coordinate iron acquisition and uptake by Pseudomonas aeruginosa(WILEY, 2017-12)Alternative sigma (σ) factors govern expression of bacterial genes in response to diverse environmental signals. In Pseudomonas aeruginosa σPvdS directs expression of genes for production of a siderophore, pyoverdine, as well as a toxin and a protease. σFpvI directs expression of a receptor for ferripyoverdine import. Expression of the genes encoding σPvdS and σFpvI is iron-regulated and an antisigma protein, FpvR20 , post-translationally controls the activities of the sigma factors in response to the amount of ferripyoverdine present. Here we show that iron represses synthesis of σPvdS to a far greater extent than σFpvI . In contrast ferripyoverdine exerts similar effects on the activities of both sigma factors. Using a combination of in vivo and in vitro assays we show that σFpvI and σPvdS have comparable affinities for, and are equally inhibited by, FpvR20 . Importantly, in the absence of ferripyoverdine the amount of FpvR20 per cell is lower than the amount of σFpvI and σPvdS , allowing basal expression of target genes that is required to activate the signalling pathway when ferripyoverdine is present. This complex interplay of transcriptional and post-translational regulation enables a co-ordinated response to ferripyoverdine but distinct responses to iron.