Publications by authors named "Siobhan Bradley"

Wines are complex mixtures of chemical compounds with broad and overlapping absorption and emission spectral features in the UV and visible spectral regions, making them challenging to study with conventional optical spectroscopic techniques. Multidimensional fluorescence spectroscopies correlate fluorescence spectra with other degrees of freedom, and have proven useful for studying complex molecular systems, offering a pathway for the analysis of wines utilising their inherent fluorescence. Here we employ steady-state excitation-emission matrix (EEM) and time-resolved fluorescence spectral measurements to investigate representative commercial white and red wine samples and a fluorescent 'model' wine base.

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  • Diketopyrrolopyrrole (DPP) derivatives are explored for their potential in singlet fission and energy upconversion due to their strong photostability and suitable energy characteristics.
  • The research utilized time-resolved electronic and IR spectroscopy to understand the excited state relaxation processes in DPP dimers with different linker structures, revealing the charge-separated (CS) state as a key intermediate that varies based on solvent and linker conditions.
  • The study concluded that while no long-lived triplet signals related to singlet fission were found, the CS state appears to serve as an alternative pathway for energy relaxation, emphasizing the importance of molecular conformation in these processes.
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Zero-dimensional (0D) quantum confinement can be achieved in perovskite materials by the confinement of electron and hole states to single PbX perovskite octahedra. In this work, 0D perovskite (CsPbBr) micro-crystals were prepared by a simple thermally-assisted solution method and thoroughly characterized. The micro-crystals show a high level of crystallinity and a high photoluminescence quantum yield of 45%.

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  • Layered perovskite films, specifically two-dimensional (2D) Ruddlesden-Popper perovskites (RPPs), exhibit better stability than traditional three-dimensional (3D) perovskites in solar cells, but suffer from lower power conversion efficiency (PCE) due to compositional inhomogeneity.
  • The addition of methylammonium chloride (MACl) has been explored to enhance PCE and stability, although its exact role in improving performance remains unclear.
  • Research utilizing advanced fluorescence and absorption techniques has shown that MACl doping reorganizes the alignment of the perovskite layers, promoting better charge carrier transport and ultimately achieving a maximum PCE of around 14.3%
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Optimizing interfacial contacts and thus electron transfer phenomena in heterogeneous electrocatalysts is an effective approach for enhancing electrocatalytic performance. Herein, we successfully synthesized ultrafine β-MoC nanoparticles confined within hollow capsules of nitrogen-doped porous carbon (β-MoC@NPCC) and found that the surface layer of molybdenum atoms was further oxidized to a single Mo-O surface layer, thus producing intimate O-Mo-C interfaces. An arsenal of complementary technologies, including XPS, atomic-resolution HAADF-STEM, and XAS analysis clearly reveals the existence of O-Mo-C interfaces for these surface-engineered ultrafine nanostructures.

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This study presents a simple one-pot synthesis method to achieve few-layered and defective Mo(S,Se) and (Mo,W)S by using supercritical water with organic reducing agents from simple and less-toxic precursors. This synthesis process is expected to be suitable for preparing other various kinds of TMD solid solutions.

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The synthesis of colloidal indium phosphide quantum dots (InP QDs) has always been plagued by difficulties arising from limited P3- sources. Being effectively restricted to the highly pyrophoric tris(trimethylsilyl) phosphine (TMS3P) creates complications for the average chemist and presents a significant risk for industrially scaled reactions. The adaptation of tris(dialkylamino) phosphines for these syntheses has garnered attention, as these new phosphines are much safer and can generate nanoparticles with competitive photoluminescence properties to those from (TMS)3P routes.

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Nanoparticles comprising three or more different metals are challenging to prepare. General methods that tackle this challenge are highly sought after as multicomponent metal nanoparticles display favorable properties in applications such as catalysis, biomedicine, and imaging. Herein, we report a practical and versatile approach for the synthesis of nanoparticles composed of up to four different metals.

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The authors describe the synthesis of water-soluble and fluorescent graphene oxide quantum dots via acid exfoliation of graphite nanoparticles. The resultant graphene oxide quantum dots (GoQDs) were then modified with folic acid. Folic acid receptors are overexpressed in cancer cells and hence can bind to functionalized graphene oxide quantum dots.

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We report a new methodology for producing monometallic or bimetallic nanoparticles confined within hollow nitrogen-doped porous carbon capsules. The capsules are derived from metal-organic framework (MOF) crystals that are coated with a shell of a secondary material comprising either a metal-tannic acid coordination polymer or a resorcinol-formaldehyde polymer. Platinum nanoparticles are optionally sandwiched between the MOF core and the shell.

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Complex scientific data is becoming the norm, many disciplines are growing immensely data-rich, and higher-dimensional measurements are performed to resolve complex relationships between parameters. Inherently multi-dimensional measurements can directly provide information on both the distributions of individual parameters and the relationships between them, such as in nuclear magnetic resonance and optical spectroscopy. However, when data originates from different measurements and comes in different forms, resolving parameter relationships is a matter of data analysis rather than experiment.

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We demonstrate microwave-induced heating of gold nanoparticles and nanorods. An appreciably higher and concentration-dependent microwave-induced heating rate was observed with aqueous dispersions of the nanomaterials as opposed to pure water and other controls. Grafted with the thermoresponsive polymer poly(N-isopropylacrylamide), these gold nanomaterials react to microwave-induced heating with a conformational change in the polymer shell, leading to particle aggregation.

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