2,914 research outputs found
Statics and Dynamics of Strongly Charged Soft Matter
Soft matter materials, such as polymers, membranes, proteins, are often
electrically charged. This makes them water soluble, which is of great
importance in technological application and a prerequisite for biological
function. We discuss a few static and dynamic systems that are dominated by
charge effects. One class comprises complexation between oppositely charged
objects, for example the adsorption of charged ions or charged polymers (such
as DNA) on oppositely charged substrates of different geometry. The second
class comprises effective interactions between similarly charged objects. Here
the main theme is to understand the experimental finding that similarly and
highly charged bodies attract each other in the presence of multi-valent
counterions. This is demonstrated using field-theoretic arguments as well as
Monte-Carlo simulations for the case of two homogeneously charged bodies.
Realistic surfaces, on the other hand, are corrugated and also exhibit
modulated charge distributions, which is important for static properties such
as the counterion-density distribution, but has even more pronounced
consequences for dynamic properties such as the counterion mobility. More
pronounced dynamic effects are obtained with highly condensed charged systems
in strong electric fields. Likewise, an electrostatically collapsed highly
charged polymer is unfolded and oriented in strong electric fields. At the end
of this review, we give a very brief account of the behavior of water at planar
surfaces and demonstrate using ab-initio methods that specific interactions
between oppositely charged groups cause ion-specific effects that have recently
moved into the focus of interest.Comment: 61 pages, 31 figures, Physics Reports (2005)-in press (high quality
figures available from authors
Critical adsorption of polyelectrolytes onto charged Janus nanospheres
Based on extensive Monte Carlo simulations and analytical considerations we
study the electrostatically driven adsorption of flexible polyelectrolyte
chains onto charged Janus nanospheres. These net-neutral colloids are composed
of two equally but oppositely charged hemispheres. The critical binding
conditions for polyelectrolyte chains are analysed as function of the radius of
the Janus particle and its surface charge density, as well as the salt
concentration in the ambient solution. Specifically for the adsorption of
finite-length polyelectrolyte chains onto Janus nanoparticles, we demonstrate
that the critical adsorption conditions drastically differ when the size of the
Janus particle or the screening length of the electrolyte are varied. We
compare the scaling laws obtained for the adsorption-desorption threshold to
the known results for uniformly charged spherical particles, observing
significant disparities. We also contrast the changes to the polyelectrolyte
chain conformations and the binding energy distributions close to the
adsorption-desorption transition for Janus nanoparticles to those for simple
spherical particles. Finally, we discuss experimentally relevant
physico-chemical systems for which our simulations results may become
important. In particular, we observe similar trends with polyelectrolyte
complexation with oppositely but heterogeneously charged proteins.Comment: 13 pages, 11 figures, RevTeX
Relaxation dynamics at different time scales in electrostatic complexes: Time-salt superposition
In this Letter we show that in the rheology of electrostatically assembled soft materials, salt concentration plays a similar role as temperature for polymer melts, and as strain rate for soft solids. We rescale linear and nonlinear rheological data of a set of model electrostatic complexes at different salt concentrations to access a range of time scales that is otherwise inaccessible. This provides new insights into the relaxation mechanisms of electrostatic complexes, which we rationalize in terms of a microscopic mechanism underlying salt-enhanced activated processe
Increased Concentration of Polyvalent Phospholipids in the Adsorption Domain of a Charged Protein
We studied the adsorption of a charged protein onto an oppositely charged
membrane, composed of mobile phospholipids of differing valence, using a
statistical-thermodynamical approach. A two-block model was employed, one block
corresponding to the protein-affected region on the membrane, referred to as
the adsorption domain, and the other to the unaffected remainder of the
membrane. We calculated the protein-induced lipid rearrangement in the
adsorption domain as arising from the interplay between the electrostatic
interactions in the system and the mixing entropy of the lipids. Equating the
electrochemical potentials of the lipids in the two blocks yields an expression
for the relations among the various lipid fractions in the adsorption domain,
indicating a sensitive dependence of lipid fraction on valence. This expression
is a result of the two-block picture but does not depend on further details of
the protein-membrane interaction. We subsequently calculated the lipid
fractions themselves using the Poisson-Boltzmann theory. We examined the
dependence of lipid enrichment, i.e., the ratio between the lipid fractions
inside and outside the adsorption domain, on various parameters such as ionic
strength and lipid valence. Maximum enrichment was found for lipid valence of
about (-3) to (-4) in physiological conditions. Our results are in qualitative
agreement with recent experimental studies on the interactions between peptides
having a domain of basic residues and membranes containing a small fraction of
the polyvalent phosphatidylinositol 4,5-bisphosphate (PIP2). This study
provides theoretical support for the suggestion that proteins adsorbed onto
membranes through a cluster of basic residues may sequester PIP2 and other
polyvalent lipids.Comment: 25 pages, 12 figure
Helical scattering and valleytronics in bilayer graphene
We describe an angularly asymmetric interface-scattering mechanism which allows to spatially separate the electrons in the two low-energy valleys of bilayer graphene. The effect occurs at electrostatically defined interfaces separating regions of different pseudospin polarization, and is associated with the helical winding of the pseudospin vector across the interface, which breaks the reflection symmetry in each valley. Electrons are transmitted with a preferred direction of up to 60° over a large energetic range in one of the valleys, and down to −60° in the other. In a Y-junction geometry, this can be used to create and detect valley polarization
Electrically Tunable Excitonic Light Emitting Diodes based on Monolayer WSe2 p-n Junctions
Light-emitting diodes are of importance for lighting, displays, optical
interconnects, logic and sensors. Hence the development of new systems that
allow improvements in their efficiency, spectral properties, compactness and
integrability could have significant ramifications. Monolayer transition metal
dichalcogenides have recently emerged as interesting candidates for
optoelectronic applications due to their unique optical properties.
Electroluminescence has already been observed from monolayer MoS2 devices.
However, the electroluminescence efficiency was low and the linewidth broad due
both to the poor optical quality of MoS2 and to ineffective contacts. Here, we
report electroluminescence from lateral p-n junctions in monolayer WSe2 induced
electrostatically using a thin boron nitride support as a dielectric layer with
multiple metal gates beneath. This structure allows effective injection of
electrons and holes, and combined with the high optical quality of WSe2 it
yields bright electroluminescence with 1000 times smaller injection current and
10 times smaller linewidth than in MoS2. Furthermore, by increasing the
injection bias we can tune the electroluminescence between regimes of
impurity-bound, charged, and neutral excitons. This system has the required
ingredients for new kinds of optoelectronic devices such as spin- and
valley-polarized light-emitting diodes, on-chip lasers, and two-dimensional
electro-optic modulators.Comment: 13 pages main text with 4 figures + 4 pages upplemental material
Bjerrum pairing correlations at charged interfaces
Electrostatic correlations play a fundamental role in aqueous solutions. In
this letter, we identify transverse and lateral correlations as two mutually
exclusive regimes. We show that the transverse regime leads to binding by
generalization of Bjerrum pair formation theory, yielding binding constants
from first-principle statistical-mechanical calculations. We compare our
theoretical predictions with experiments on charged membranes and Langmuir
monolayers and find good agreement. We contrast our approach with existing
theories in the strong-coupling limit and on charged modulated interfaces, and
discuss different scenarios that lead to charge reversal and equal-sign
attraction by macro-ions.Comment: 7 pages, 4 figure
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