Vapour-liquid coexistence in many-body dissipative particle dynamics

Many-body dissipative particle dynamics is constructed to exhibit vapour-liquid coexistence, with a sharp interface, and a vapour phase of vanishingly small density. In this form, the model is an unusual example of a soft-sphere liquid with a potential energy built out of local-density dependent one-particle self energies. The application to fluid mechanics problems involving free surfaces is illustrated by simulation of a pendant drop.Comment: 8 pages, 6 figures, revtex

Reproduction Portrait Photograph of Abraham Lincoln

The object is a reproduction of a portrait photograph of Abraham Lincoln, taken by Christopher S. German in 1861. [Ref; O-43.]https://scholarsjunction.msstate.edu/fvw-photographs/1529/thumbnail.jp

Hydrodynamic bubble coarsening in off-critical vapour-liquid phase separation

Late-stage coarsening in off-critical vapour-liquid phase separation is re-examined. In the limit of bubbles of vapour distributed throughout a continuous liquid phase, it is argued that coarsening proceeds via inertial hydrodynamic bubble collapse. This replaces the Lifshitz-Slyozov-Wagner mechanism seen in binary liquid mixtures. The arguments are strongly supported by simulations in two dimensions using a novel single-component soft sphere fluid.Comment: 5 pages, 3 figures, revtex3.

Hydrodynamic interactions and Brownian forces in colloidal suspensions: Coarse-graining over time and length-scales

We describe in detail how to implement a coarse-grained hybrid Molecular Dynamics and Stochastic Rotation Dynamics simulation technique that captures the combined effects of Brownian and hydrodynamic forces in colloidal suspensions. The importance of carefully tuning the simulation parameters to correctly resolve the multiple time and length-scales of this problem is emphasized. We systematically analyze how our coarse-graining scheme resolves dimensionless hydrodynamic numbers such as the Reynolds number, the Schmidt number, the Mach number, the Knudsen number, and the Peclet number. The many Brownian and hydrodynamic time-scales can be telescoped together to maximize computational efficiency while still correctly resolving the physically relevant physical processes. We also show how to control a number of numerical artifacts, such as finite size effects and solvent induced attractive depletion interactions. When all these considerations are properly taken into account, the measured colloidal velocity auto-correlation functions and related self diffusion and friction coefficients compare quantitatively with theoretical calculations. By contrast, these calculations demonstrate that, notwithstanding its seductive simplicity, the basic Langevin equation does a remarkably poor job of capturing the decay rate of the velocity auto-correlation function in the colloidal regime, strongly underestimating it at short times and strongly overestimating it at long times. Finally, we discuss in detail how to map the parameters of our method onto physical systems, and from this extract more general lessons that may be relevant for other coarse-graining schemes such as Lattice Boltzmann or Dissipative Particle Dynamics.Comment: 31 pages, 14 figure

Exploring tandem ruthenium-catalyzed hydrogen transfer and SNAr chemistry

A hydrogen-transfer strategy for the catalytic functionalization of benzylic alcohols via electronic arene activation, accessing a diverse range of bespoke diaryl ethers and aryl amines in excellent isolated yields (38 examples, 70% average yield), is reported. Taking advantage of the hydrogen-transfer approach, the oxidation level of the functionalized products can be selected by judicious choice of simple and inexpensive additives

Beware of density dependent pair potentials

Density (or state) dependent pair potentials arise naturally from coarse-graining procedures in many areas of condensed matter science. However, correctly using them to calculate physical properties of interest is subtle and cannot be uncoupled from the route by which they were derived. Furthermore, there is usually no unique way to coarse-grain to an effective pair potential. Even for simple systems like liquid Argon, the pair potential that correctly reproduces the pair structure will not generate the right virial pressure. Ignoring these issues in naive applications of density dependent pair potentials can lead to an apparent dependence of thermodynamic properties on the ensemble within which they are calculated, as well as other inconsistencies. These concepts are illustrated by several pedagogical examples, including: effective pair potentials for systems with many-body interactions, and the mapping of charged (Debye-H\"{u}ckel) and uncharged (Asakura-Oosawa) two-component systems onto effective one-component ones.Comment: 22 pages, uses iopart.cls and iopart10.clo; submitted to Journal of Physics Condensed Matter, special issue in honour of professor Jean-Pierre Hanse

Macromolecular theory of solvation and structure in mixtures of colloids and polymers

The structural and thermodynamic properties of mixtures of colloidal spheres and non-adsorbing polymer chains are studied within a novel general two-component macromolecular liquid state approach applicable for all size asymmetry ratios. The dilute limits, when one of the components is at infinite dilution but the other concentrated, are presented and compared to field theory and models which replace polymer coils with spheres. Whereas the derived analytical results compare well, qualitatively and quantitatively, with mean-field scaling laws where available, important differences from ``effective sphere'' approaches are found for large polymer sizes or semi-dilute concentrations.Comment: 23 pages, 10 figure

Non-monotonic variation with salt concentration of the second virial coefficient in protein solutions

The osmotic virial coefficient $B_2$ of globular protein solutions is calculated as a function of added salt concentration at fixed pH by computer simulations of the ``primitive model''. The salt and counter-ions as well as a discrete charge pattern on the protein surface are explicitly incorporated. For parameters roughly corresponding to lysozyme, we find that $B_2$ first decreases with added salt concentration up to a threshold concentration, then increases to a maximum, and then decreases again upon further raising the ionic strength. Our studies demonstrate that the existence of a discrete charge pattern on the protein surface profoundly influences the effective interactions and that non-linear Poisson Boltzmann and Derjaguin-Landau-Verwey-Overbeek (DLVO) theory fail for large ionic strength. The observed non-monotonicity of $B_2$ is compared to experiments. Implications for protein crystallization are discussed.Comment: 43 pages, including 17 figure

Quantum feedback with weak measurements

The problem of feedback control of quantum systems by means of weak measurements is investigated in detail. When weak measurements are made on a set of identical quantum systems, the single-system density matrix can be determined to a high degree of accuracy while affecting each system only slightly. If this information is fed back into the systems by coherent operations, the single-system density matrix can be made to undergo an arbitrary nonlinear dynamics, including for example a dynamics governed by a nonlinear Schr\"odinger equation. We investigate the implications of such nonlinear quantum dynamics for various problems in quantum control and quantum information theory, including quantum computation. The nonlinear dynamics induced by weak quantum feedback could be used to create a novel form of quantum chaos in which the time evolution of the single-system wave function depends sensitively on initial conditions.Comment: 11 pages, TeX, replaced to incorporate suggestions of Asher Pere

Extending colonic mucosal microbiome analysis - Assessment of colonic lavage as a proxy for endoscopic colonic biopsies

This study was supported through GI Research funds and MRC Grant Ref: MR/M00533X/1 to GH.Peer reviewedPublisher PD