685 research outputs found
Hard Spheres in Vesicles: Curvature-Induced Forces and Particle-Induced Curvature
We explore the interplay of membrane curvature and nonspecific binding due to
excluded-volume effects among colloidal particles inside lipid bilayer
vesicles. We trapped submicron spheres of two different sizes inside a
pear-shaped, multilamellar vesicle and found the larger spheres to be pinned to
the vesicle's surface and pushed in the direction of increasing curvature. A
simple model predicts that hard spheres can induce shape changes in flexible
vesicles. The results demonstrate an important relationship between the shape
of a vesicle or pore and the arrangement of particles within it.Comment: LaTeX with epsfig; ps available at
http://dept.physics.upenn.edu/~nelson/index.shtml Phys Rev Lett in press
(1997
Depletion forces near curved surfaces
Based on density functional theory the influence of curvature on the
depletion potential of a single big hard sphere immersed in a fluid of small
hard spheres with packing fraction \eta_s either inside or outside of a hard
spherical cavity of radius R_c is calculated. The relevant features of this
potential are analyzed as function of \eta_s and R_c. There is a very slow
convergence towards the flat wall limit R_c \to \infty. Our results allow us to
discuss the strength of depletion forces acting near membranes both in normal
and lateral directions and to make contact with recent experimental results
Understanding depletion forces beyond entropy
The effective interaction energy of a colloidal sphere in a suspension
containing small amounts of non-ionic polymers and a flat glass surface has
been measured and calculated using total internal reflection microscopy (TIRM)
and a novel approach within density functional theory (DFT), respectively.
Quantitative agreement between experiment and theory demonstrates that the
resulting repulsive part of the depletion forces cannot be interpreted entirely
in terms of entropic arguments but that particularly at small distances
( 100 nm) attractive dispersion forces have to be taken into account
Radiocarbon dating of methane and carbon dioxide evaded from a temperate peatland stream
Streams draining peatlands export large quantities of carbon in different chemical forms and
are an important part of the carbon cycle. Radiocarbon (14C) analysis/dating provides unique
information on the source and rate that carbon is cycled through ecosystems, as has recently
been demonstrated at the air-water interface through analysis of carbon dioxide (CO2) lost
from peatland streams by evasion (degassing). Peatland streams also have the potential to
release large amounts of methane (CH4) and, though 14C analysis of CH4 emitted by ebullition
(bubbling) has been previously reported, diffusive emissions have not. We describe methods
that enable the 14C analysis of CH4 evaded from peatland streams. Using these methods, we
investigated the 14C age and stable carbon isotope composition of both CH4 and CO2 evaded
from a small peatland stream draining a temperate raised mire. Methane was aged between
1617-1987 years BP, and was much older than CO2 which had an age range of 303-521 years
BP. Isotope mass balance modelling of the results indicated that the CO2 and CH4 evaded
from the stream were derived from different source areas, with most evaded CO2 originating
from younger layers located nearer the peat surface compared to CH4. The study demonstrates
the insight that can be gained into peatland carbon cycling from a methodological
development which enables dual isotope (14C and 13C) analysis of both CH4 and CO2 collected
at the same time and in the same way
Direct measurements of the effects of salt and surfactant on interaction forces between colloidal particles at water-oil interfaces
The forces between colloidal particles at a decane-water interface, in the
presence of low concentrations of a monovalent salt (NaCl) and of the
surfactant sodium dodecylsulfate (SDS) in the aqueous subphase, have been
studied using laser tweezers. In the absence of electrolyte and surfactant,
particle interactions exhibit a long-range repulsion, yet the variation of the
interaction for different particle pairs is found to be considerable. Averaging
over several particle pairs was hence found to be necessary to obtain reliable
assessment of the effects of salt and surfactant. It has previously been
suggested that the repulsion is consistent with electrostatic interactions
between a small number of dissociated charges in the oil phase, leading to a
decay with distance to the power -4 and an absence of any effect of electrolyte
concentration. However, the present work demonstrates that increasing the
electrolyte concentration does yield, on average, a reduction of the magnitude
of the interaction force with electrolyte concentration. This implies that
charges on the water side also contribute significantly to the electrostatic
interactions. An increase in the concentration of SDS leads to a similar
decrease of the interaction force. Moreover the repulsion at fixed SDS
concentrations decreases over longer times. Finally, measurements of three-body
interactions provide insight into the anisotropic nature of the interactions.
The unique time-dependent and anisotropic interactions between particles at the
oil-water interface allow tailoring of the aggregation kinetics and structure
of the suspension structure.Comment: Submitted to Langmui
Self-assembly of Microcapsules via Colloidal Bond Hybridization and Anisotropy
Particles with directional interactions are promising building blocks for new
functional materials and may serve as models for biological structures.
Mutually attractive nanoparticles that are deformable due to flexible surface
groups, for example, may spontaneously order themselves into strings, sheets
and large vesicles. Furthermore, anisotropic colloids with attractive patches
can self-assemble into open lattices and colloidal equivalents of molecules and
micelles. However, model systems that combine mutual attraction, anisotropy,
and deformability have---to the best of our knowledge---not been realized.
Here, we synthesize colloidal particles that combine these three
characteristics and obtain self-assembled microcapsules. We propose that mutual
attraction and deformability induce directional interactions via colloidal bond
hybridization. Our particles contain both mutually attractive and repulsive
surface groups that are flexible. Analogous to the simplest chemical bond,
where two isotropic orbitals hybridize into the molecular orbital of H2, these
flexible groups redistribute upon binding. Via colloidal bond hybridization,
isotropic spheres self-assemble into planar monolayers, while anisotropic
snowman-like particles self-assemble into hollow monolayer microcapsules. A
modest change of the building blocks thus results in a significant leap in the
complexity of the self-assembled structures. In other words, these relatively
simple building blocks self-assemble into dramatically more complex structures
than similar particles that are isotropic or non-deformable
Free energy of colloidal particles at the surface of sessile drops
The influence of finite system size on the free energy of a spherical
particle floating at the surface of a sessile droplet is studied both
analytically and numerically. In the special case that the contact angle at the
substrate equals a capillary analogue of the method of images is
applied in order to calculate small deformations of the droplet shape if an
external force is applied to the particle. The type of boundary conditions for
the droplet shape at the substrate determines the sign of the capillary
monopole associated with the image particle. Therefore, the free energy of the
particle, which is proportional to the interaction energy of the original
particle with its image, can be of either sign, too. The analytic solutions,
given by the Green's function of the capillary equation, are constructed such
that the condition of the forces acting on the droplet being balanced and of
the volume constraint are fulfilled. Besides the known phenomena of attraction
of a particle to a free contact line and repulsion from a pinned one, we
observe a local free energy minimum for the particle being located at the drop
apex or at an intermediate angle, respectively. This peculiarity can be traced
back to a non-monotonic behavior of the Green's function, which reflects the
interplay between the deformations of the droplet shape and the volume
constraint.Comment: 24 pages, 19 figure
Phase behaviour of additive binary mixtures in the limit of infinite asymmetry
We provide an exact mapping between the density functional of a binary
mixture and that of the effective one-component fluid in the limit of infinite
asymmetry. The fluid of parallel hard cubes is thus mapped onto that of
parallel adhesive hard cubes. Its phase behaviour reveals that demixing of a
very asymmetric mixture can only occur between a solvent-rich fluid and a
permeated large particle solid or between two large particle solids with
different packing fractions. Comparing with hard spheres mixtures we conclude
that the phase behaviour of very asymmetric hard-particle mixtures can be
determined from that of the large component interacting via an adhesive-like
potential.Comment: Full rewriting of the paper (also new title). 4 pages, LaTeX, uses
revtex, multicol, epsfig, and amstex style files, to appear in Phys. Rev. E
(Rapid Comm.
A coil-globule transition of a semiflexible polymer driven by the addition of spherical particles
The phase behaviour of a single large semiflexible polymer immersed in a
suspension of spherical particles is studied. All interactions are simple
excluded volume interactions and the diameter of the spherical particles is an
order of magnitude larger than the diameter of the polymer. The spherical
particles induce a quite long ranged depletion attraction between the segments
of the polymer and this induces a continuous coil-globule transition in the
polymer. This behaviour gives an indication of the condensing effect of
macromolecular crowding on DNA.Comment: 12 pages, 4 figure
The low temperature interface between the gas and solid phases of hard spheres with a short-ranged attraction
At low temperature, spheres with a very short-ranged attraction exist as a
close-packed solid coexisting with an infinitely dilute gas. We find that the
ratio of the interfacial tension between these two phases to the thermal energy
diverges as the range of the attraction goes to zero. The large tensions when
the interparticle attractions are short-ranged may be why globular proteins
only crystallise over a narrow range of conditions.Comment: 6 pages, no figures (v2 has change of notation to agree with that of
Stell
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