Bulk simulation of polar liquids in spherical symmetry.

Molecular simulations of strongly coupled dipolar systems of varying size have been carried out, using particles confined inside a dielectric cavity and an image charge approach to treat the dielectric response from the surroundings. A simple method using penalty functions was employed to create an isotropic and homogeneous distribution of particles inside the cavity. The dielectric response of the molecular system was found to increase as the number of particles N was increased. Nevertheless, a significant surface effect remained even for the largest systems (N=10,000), manifesting itself through a decrease in the dielectric constant of the system as the confining surface was approached. The surface effect was significantly reduced by using a negative dielectric constant of the surrounding dielectric medium, although accomplishing a full dielectric solvation of the molecular system was not possible

Nondielectric long-range solvation of polar liquids in cubic symmetry

Long-range solvation properties of strongly coupled dipolar systems simulated using the Ewald and reaction field methods are assessed by using electric fluctuation formulas for a dielectric medium. Some components of the fluctuating electric multipole moments are suppressed, whereas other components are favored as the boundary of the simulation box is approached. An analysis of electrostatic interactions in a periodic cubic system suggests that these structural effects are due to the periodicity embedded in the Ewald method. Furthermore, the results obtained using the reaction field method are very similar to those obtained using the Ewald method, an effect which we attribute to the use of toroidal boundary conditions in the former case. Thus, the long-range solvation properties of polar liquids simulated using either of the two methods are nondielectric in their character. (C) 2009 American Institute of Physics. [doi:10.1063/1.3250941

Molecular data suggest long-term in Situ Antarctic persistence within Antarctica's most speciose plant genus, Schistidium

© 2018 Biersma, Jackson, Stech, Griffiths, Linse and Convey. From glacial reconstructions it is clear that Antarctic terrestrial life must have been extremely limited throughout Quaternary glacial periods. In contrast, recent biological studies provide clear evidence for long-term in situ persistence throughout glacial times within most extant Antarctic faunal and several microbial groups. However, even now, the evolutionary history of the Antarctic flora-despite playing major role in Antarctic ecosystems-remains poorly studied. We assessed the diversity, richness and relative age divergences within Schistidium (Grimmiaceae, Bryophyta), the most species-rich plant genus in the Antarctic, as well as the plant genus containing most Antarctic endemic species. We applied phylogenetic and molecular dating methods based on nuclear ribosomal Internal Transcribed Spacer sequences, including all known Antarctic Schistidium species with available sample material. We additionally investigated the continent-wide genetic diversity within the most common Antarctic representative of the genus-the endemic species Schistidium antarctici-and performed preliminary phylogeographic analyses of the bipolar species Schistidium rivulare. Most previously described Antarctic Schistidium species were genetically distinct, confirming their specific status. Interspecific divergences of all species took place at least ~1 Mya, suggesting a likely in situ persistence in Antarctica for (at least) all endemic Schistidium species. The widespread endemic species, Schistidium antarctici, diverged from other Antarctic congeners in the late Miocene, thereby revealing the oldest extant plant species currently known in Antarctica, and providing increasing support for the hypothesis of vegetation survival through multiple glacial periods. Within S. antarctici we identified several distinct clades dividing the eastern Antarctic Peninsula and Scotia Arc islands from the western Antarctic Peninsula and all continental locations. This suggests that the mountainous spine on the Antarctic Peninsula forms a strong barrier to gene flow in this species, while increased genetic diversity in the northern Maritime Antarctic indicates likely glacial refugia in this area. This study provides an important first step toward assessing the diversity and evolutionary history of the most speciose moss genus in the Antarctic. The multi-million year presence of several endemic species contributes to studies on their adaptive potential to survive climate change over both historical and contemporary timescales.NERC STUDENTSHIP NE/K50094X/

Low genetic variation between South American and Antarctic populations of the bank-forming moss Chorisodontium aciphyllum (Dicranaceae)

The Antarctic–South American bank-forming moss Chorisodontium aciphyllum is known for having the oldest sub-fossils of any extant plant in Antarctica as well as extreme survival abilities, making it a candidate species for possible long-term survival in Antarctica. Applying phylogeographic and population genetic methods using the plastid markers trnL-F and rps4 and the nuclear internal transcribed spacer, we investigated the genetic diversity within C. aciphyllum throughout its range. Low genetic variation was found in all loci, both between and within Antarctic and southern South American populations, suggesting a relatively recent (likely within the last million years) colonization of this moss to the Antarctic, as well as a likely severe bottleneck during Pleistocene glaciations in southern South America. We also performed a simple atmospheric transfer modeling approach to study potential colonization rates of small (microscopic/microbial) or spore-dispersed organisms (such as many mosses and lichens). These suggested that the northern Antarctic Peninsula shows potentially regular connectivity from southern South America, with air masses transferring, particularly southbound, between the two regions. We found elevated genetic variation of C. aciphyllum in Elephant Island, also the location of the oldest known moss banks (> 5500 years), suggesting this location to be a genetic hotspot for this species in the Antarctic.This research was funded by a Natural Environment Research Council (NERC) Ph.D. studentship (ref. NE/K50094X/1) to E.M.B. and supported by NERC core funding to the BAS Biodiversity, Evolution and Adaptation Team

On the fluid-fluid phase separation in charged-stabilized colloidal suspensions

We develop a thermodynamic description of particles held at a fixed surface potential. This system is of particular interest in view of the continuing controversy over the possibility of a fluid-fluid phase separation in aqueous colloidal suspensions with monovalent counterions. The condition of fixed surface potential allows in a natural way to account for the colloidal charge renormalization. In a first approach, we assess the importance of the so called ``volume terms'', and find that in the absence of salt, charge renormalization is sufficient to stabilize suspension against a fluid-fluid phase separation. Presence of salt, on the other hand, is found to lead to an instability. A very strong dependence on the approximations used, however, puts the reality of this phase transition in a serious doubt. To further understand the nature of the instability we next study a Jellium-like approximation, which does not lead to a phase separation and produces a relatively accurate analytical equation of state for a deionized suspensions of highly charged colloidal spheres. A critical analysis of various theories of strongly asymmetric electrolytes is presented to asses their reliability as compared to the Monte Carlo simulations

Global biogeographic patterns in bipolar moss species

A bipolar disjunction is an extreme, yet common, biogeographic pattern in non-vascular plants, yet its underlyingmechanisms (vicariance or long-distance dispersal), origin and timing remain poorly understood. Here, combining a large-scale population dataset and multiple dating analyses, we examine the biogeography of four bipolar Polytrichales mosses, common to the Holarctic (temperate and polar Northern Hemisphere regions) and the Antarctic region (Antarctic, sub-Antarctic, southern South America) and other Southern Hemisphere (SH) regions. Our data reveal contrasting patterns, for three species were of Holarctic origin, with subsequent dispersal to the SH, while one, currently a particularly common species in the Holarctic (Polytrichum juniperinum), diversified in the Antarctic region and from here colonized both the Holarctic and other SH regions. Our findings suggest long-distance dispersal as the driver of bipolar disjunctions. We find such inter-hemispheric dispersals are rare, occurring on multi-million-year timescales. High-altitude tropical populations did not act as trans-equatorial 'steppingstones', but rather were derived from later dispersal events. All arrivals to the Antarctic region occurred well before the Last Glacial Maximum and previous glaciations, suggesting that, despite the harsh climate during these past glacial maxima, plants have had a much longer presence in this southern region than previously thought.Peer reviewe

Poisson-Boltzmann Theory of Charged Colloids: Limits of the Cell Model for Salty Suspensions

Thermodynamic properties of charge-stabilised colloidal suspensions are commonly modeled by implementing the mean-field Poisson-Boltzmann (PB) theory within a cell model. This approach models a bulk system by a single macroion, together with counterions and salt ions, confined to a symmetrically shaped, electroneutral cell. While easing solution of the nonlinear PB equation, the cell model neglects microion-induced correlations between macroions, precluding modeling of macroion ordering phenomena. An alternative approach, avoiding artificial constraints of cell geometry, maps a macroion-microion mixture onto a one-component model of pseudo-macroions governed by effective interactions. In practice, effective-interaction models are usually based on linear screening approximations, which can accurately describe nonlinear screening only by incorporating an effective (renormalized) macroion charge. Combining charge renormalization and linearized PB theories, in both the cell model and an effective-interaction (cell-free) model, we compute osmotic pressures of highly charged colloids and monovalent microions over a range of concentrations. By comparing predictions with primitive model simulation data for salt-free suspensions, and with predictions of nonlinear PB theory for salty suspensions, we chart the limits of both the cell model and linear-screening approximations in modeling bulk thermodynamic properties. Up to moderately strong electrostatic couplings, the cell model proves accurate in predicting osmotic pressures of deionized suspensions. With increasing salt concentration, however, the relative contribution of macroion interactions grows, leading predictions of the cell and effective-interaction models to deviate. No evidence is found for a liquid-vapour phase instability driven by monovalent microions. These results may guide applications of PB theory to soft materials.Comment: 27 pages, 5 figures, special issue of Journal of Physics: Condensed Matter on "Classical density functional theory methods in soft and hard matter

Charge Renormalization, Effective Interactions, and Thermodynamics of Deionized Colloidal Suspensions

Thermodynamic properties of charge-stabilised colloidal suspensions depend sensitively on the effective charge of the macroions, which can be substantially lower than the bare charge in the case of strong counterion-macroion association. A theory of charge renormalization is proposed, combining an effective one-component model of charged colloids with a thermal criterion for distinguishing between free and associated counterions. The theory predicts, with minimal computational effort, osmotic pressures of deionized suspensions of highly charged colloids in close agreement with large-scale simulations of the primitive model.Comment: 15 pages, 7 figure