Tristan G. A. Youngs

Structure and dynamics of aqueous 2-propanol: a THz-TDS, NMR and neutron diffraction study

Aqueous liquid mixtures, in particular, those involving amphiphilic species, play an important role in many physical, chemical and biological processes. Of particular interest are alcohol/water mixtures; however, the structural dynamics of such systems are still not fully understood. Herein, a combination of terahertz time-domain spectroscopy (THz-TDS) and NMR relaxation time analysis has been applied to investigate 2-propanol/water mixtures across the entire composition range; while neutron diffraction studies have been carried out at two specific concentrations. Excellent agreement is seen between the techniques with a maximum in both the relative absorption coefficient and the activation energy to molecular motion occurring at ∼90 mol% H2O. Furthermore, this is the same value at which well-established excess thermodynamic functions exhibit a maximum/minimum. Additionally, both neutron diffraction and THz-TDS have been used to provide estimates of the size of the hydration shell around 2-propanol in solution. Both methods determine that between 4 and 5 H2O molecules per 2-propanol are found in the 2-propanol/water clusters at 90 mol% H2O. Based on the acquired data, a description of the structure of 2-propanol/water across the composition range is presented.

Structural, electronic and kinetic properties of the phase-change material Ge2Sb2Te5 in the liquid state.

Phase-change materials exhibit fast and reversible transitions between an amorphous and a crystalline state at high temperature. The two states display resistivity contrast, which is exploited in phase-change memory devices. The technologically most important family of phase-change materials consists of Ge-Sb-Te alloys. In this work, we investigate the structural, electronic and kinetic properties of liquid Ge2Sb2Te5 as a function of temperature by a combined experimental and computational approach. Understanding the properties of this phase is important to clarify the amorphization and crystallization processes. We show that the structural properties of the models obtained from ab initio and reverse Monte Carlo simulations are in good agreement with neutron and X-ray diffraction experiments. We extract the kinetic coefficients from the molecular dynamics trajectories and determine the activation energy for viscosity. The obtained value is shown to be fully compatible with our viscosity measurements.

Neutron Scattering of Aromatic and Aliphatic Liquids.

Abstract Organic solvents, such as cyclohexane, cyclohexene, methylcyclohexane, benzene and toluene, are widely used as both reagents and solvents in industrial processes. Despite the ubiquity of these liquids, the local structures that govern the chemical properties have not been studied extensively. Herein, we report neutron diffraction measurements on liquid cyclohexane, cyclohexene, methylcyclohexane, benzene and toluene at 298 K to obtain a detailed description of the local structure in these compounds. The radial distribution functions of the centres of the molecules, as well as the partial distribution functions for the double bond for cyclohexene and methyl group for methylcyclohexane and toluene have been calculated. Additionally, probability density functions and angular radial distribution functions were extracted to provide a full description of the local structure within the chosen liquids. Structural motifs are discussed and compared for all liquids, referring specifically to the functional group and aromaticity present in the different liquids.

Structure of ionic liquids with amino acid anions via neutron diffraction

The liquid structures of the ionic liquids 1-ethyl-3-methylimidazolium alaninate and 1-ethyl-3-methylimidazolium serinate are fully elucidated through the application of neutron diffraction techniques. We observe significant direct interaction between anions, particularly in the case of the serinate ionic liquid which is strongly hydrogen bonding between its hydroxyl and carboxylate groups, and is attributed the significant increase in viscosity of the neat liquid to this structural feature. Minor differences in the elucidated interactions are present between the R and S forms of the anions.

Solvation Structure of Uracil in Ionic Liquids.

The local solvation environment of uracil dissolved in the ionic liquid 1-ethyl-3-methylimidazolium acetate has been studied using neutron diffraction techniques. At solvent:solute (ionic liquid:uracil) ratios of 3:1 and 2:1, little perturbation of the ion-ion correlations compared to those of the neat ionic liquid are observed. We find that solvation of the uracil is driven predominantly by the acetate anion of the solvent. While short distance correlations exist between uracil and the imidazolium cation, the geometry of these contacts suggest that they cannot be considered as hydrogen bonds, in contrast to other studies by Araújo et al. (J. M. Araújo, A. B. Pereiro, J. N. Canongia-Lopes, L. P. Rebelo, I. M. Marrucho, J. Phys. Chem. B 2013, 117, 4109-4120). Nevertheless, this combination of interactions of the solute with both the cation and anion components of the solvents helps explain the high solubility of the nucleobase in this media. In addition, favourable uracil-uracil contacts are observed, of similar magnitude to those between cation and uracil, and are also likely to aid dissolution.

Micrometer-sized Water Ice Particles for Planetary Science Experiments: Influence of Surface Structure on Collisional Properties

Models and observations suggest that ice-particle aggregation at and beyond the snowline dominates the earliest stages of planet-formation, which therefore is subject to many laboratory studies. However, the pressure-temperature gradients in proto-planetary disks mean that the ices are constantly processed, undergoing phase changes between different solid phases and the gas phase. Open questions remain as to whether the properties of the icy particles themselves dictate collision outcomes and therefore how effectively collision experiments reproduce conditions in pro- toplanetary environments. Previous experiments often yielded apparently contradictory results on collision outcomes, only agreeing in a temperature dependence setting in above

Determination of toluene hydrogenation kinetics with neutron diffraction.

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Confinement effects on the benzene orientational structure

210 K. By exploiting the unique capabilities of the NIMROD neutron scattering instrument, we characterized the bulk and surface structure of icy particles used in collision experiments, and studied how these structures alter as a function of temperature at a constant pressure of around 30 mbar. Our icy grains, formed under liquid nitrogen, undergo changes in the crystalline ice-phase, sublimation, sintering and surface pre-melting as they are heated from 103 to 247 K. An increase in the thickness of the diffuse surface layer from

The structure of ethylbenzene, styrene and phenylacetylene determined by total neutron scattering

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Formation of Methane Hydrate in the Presence of Natural and Synthetic Nanoparticles

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