We report a study of the cholesteric phase in monodisperse suspensions of the rodlike virus fd sterically stabilized with the polymer polyethylene glycol (PEG). After coating the virus with neutral polymers, the phase diagram and nematic order parameter of the fd-PEG system then become independent of ionic strength. Surprisingly, the fd-PEG suspensions not only continue to exhibit a cholesteric phase, which means that the grafted polymer does not screen all chiral interactions between rods, but paradoxically the cholesteric pitch of this sterically stabilized fd-PEG system varies with ionic strength. Furthermore, we observe that the cholesteric pitch decreases with increasing viral contour length, in contrast to theories which predict the opposite trend. Different models of the origin of chirality in colloidal liquid crystals are discussed.
We present an experimental study of the isotropic-nematic phase transition in an aqueous mixture of charged semi-flexible rods (fd virus) and neutral polymer (Dextran). A complete phase diagram is measured as a function of ionic strength and polymer molecular weight. At high ionic strength we find that adding polymer widens the isotropic-nematic coexistence region with polymers preferentially partitioning into the isotropic phase, while at low ionic strength the added polymer has no effect on the phase transition. The nematic order parameter is determined from birefringence measurements and is found to be independent of polymer concentration (or equivalently the strength of attraction). The experimental results are compared with the existing theoretical predictions for the isotropic-nematic transition in rods with attractive interactions.
We report the direct visualization at the scale of single particles of mass transport between smectic layers, also called permeation, in a suspension of rod-like viruses. Self-diffusion takes place preferentially in the direction normal to the smectic layers, and occurs by quasi-quantized steps of one rod length. The diffusion rate corresponds with the rate calculated from the diffusion in the nematic state with a lamellar periodic ordering potential that is obtained experimentally.Since the pioneering work of Onsager on the entropy driven phase transition to a liquid crystalline state [1], the structure and the phase behavior of complex fluids containing anisotropic particles with hard core interactions has been a subject of considerable interest, both theoretically [2] and experimentally [3]. Understanding of the particle mobility in the different liquid crystalline phases is more recent [4]. In experiments various methods have been applied to obtain the ensemble averaged selfdiffusion coefficients in thermotropic [5] and amphiphilic [6] liquid crystals, block copolymer [7] and colloidal systems [8]. Only a few studies have been done where dynamical phenomena are probed at the scale of a single anisotropic particle: the Brownian motion of an isolated colloidal ellipsoid in confined geometry [9] and the selfdiffusion in a nematic phase formed by rod-like viruses [10] represent two recent examples. In the latter case, the diffusion parallel (D ) and perpendicular (D ⊥ ) to the average rod orientation (the director) has been measured, showing an increase of the ratio D /D ⊥ with particle concentration. Knowledge of the dynamics at the single particle level is fundamental for understanding the physics of mesophases with spatial order like the smectic (lamellar) phase of rod-like particles. In this mesophase the particle density is periodic in one dimension parallel to the long axis of the rods, while the interparticle correlations perpendicular to this axis are short-ranged (fluid-like order). For parallel diffusion to take place, the rods need to jump between adjacent smectic layers, overcoming an energy barrier related to the smectic order parameter [11]. This process of interlayer diffusion, or permeation, was first predicted by Helfrich [12]. In this Letter, we use video fluorescence microscopy to monitor the dynamics of individual labeled colloidal rods in the background of a smectic mesophase formed by identical but unlabeled rods. In this way we directly observe permeation of single rods in adjacent layers. As in the nematic phase, self-diffusion in a smectic phase is anisotropic: the diffusion through the smectic layers is shown here to be much faster than the diffusion within each liquid-like layer, i.e. D /D ⊥ ≫ 1, in contrast to thermotropic systems. Moreover, since the individual rod positions within the layer are monitored, the potential barrier for permeation is straightly determined for the first time. The permeation can then be . The layer spacing is L ≃ 0.9 µm. (b) Displacement of a given particle...
We report a study on charged, filamentous virus called M13, whose suspensions in water exhibit a chiral nematic (cholesteric) phase. In spite of the right-handed helicity of the virus, a left-handed phase helicity is found, with a cholesteric pitch which increases with temperature and ionic strength. Several sources of chirality can be devised in the system, ranging from the subnanometer to the micrometer length scale. Here an explanation is proposed for the microscopic origin of the cholesteric organization, which arises from the helical arrangement of coat proteins on the virus surface. The phase organization is explained as the result of the competition between contributions of opposite handedness, deriving from best packing of viral particles and electrostatic interparticle repulsions. This hypothesis is supported by calculations based on a coarse-grained representation of the virus.
We report a study of colloidal suspensions of highly monodisperse semiflexible chiral rodlike viruses, denoted fd, in the range of high concentrations. Small angle x-ray scattering experiments reveal the existence of two hexagonal phases: the first one is crystalline and the second one is hexatic columnar, as shown by its short-range positional order. The suspension of rodlike viruses is the first experimental system showing the whole phase sequence with increasing particle concentration theoretically predicted for systems of hard rods, ranging from the chiral nematic via the smectic to columnar and crystalline phases.
We report a study of the growth and of the orientation of thin open supported columnar liquid crystal films by thermal annealing. We show that there is a competition between planar and homeotropic orientations (columns respectively oriented parallel and perpendicular to the solid substrate) of the liquid crystal, which can be controlled by the kinetics of annealing. A model based on the different surface tensions of the system is proposed to account for the experimental observations. Such a control of the alignment opens the way towards discotics based optoelectronic devices.
Aqueous dispersions of exfoliated, bile-salt stabilized single-wall carbon nanotubes exhibit a first order transition to a nematic liquid-crystalline phase. The nematic phase presents itself in the form of micron-sized nematic droplets also known as tactoids, freely floating in the isotropic host dispersion. The nematic droplets are spindle shaped and have an aspect ratio of about four, irrespective of their size. We attribute this to a director field that is uniform rather than bipolar, which is confirmed by polarization microscopy. It follows that the ratio of the anchoring strength and the surface tension must be about four, which is quite larger than predicted theoretically but in line with earlier observations of bipolar tactoids. From the scatter in the data we deduce that the surface tension of the coexisting isotropic and nematic phases must be extremely low, that is, of the order of nN/m. Carbon nanotubes or CNTs are colloidal particles with a very large aspect ratio, typically in the range from many tens to hundreds up to even thousands. Hence, it is not surprising that, provided they are properly stabilized against aggregation, fluid dispersions containing CNTs exhibit an Onsagertype isotropic-nematic transition ͓1-6͔. This happens at concentrations in excess of a critical value that depends on the aspect ratio of the rods. The relevant concentration scale here is the volume or packing fraction because the driving force for the spontaneous alignment is the anisotropic volume exclusion between the particles. For the nematic to become stable the volume fraction of CNTs should be in excess of a few times the reciprocal of some average of their aspect ratios ͓7͔. It follows that the nematic transition must occur at very low concentrations of, say, one per cent of CNTs. This, by and large, is in agreement with experimental observation, allowing for instance for the effects of polydispersity ͓1-6͔.Often, before isotropic-nematic phase separation occurs on a macroscopic scale in dispersions of elongated colloidal particles, the nematic phase establishes itself in the form of droplets called tactoids. Tactoids have been observed in many dispersions, such as tobacco mosaic virus ͓8,9͔, boehmite rods ͓10͔, poly͑butyl glutamate͒, self-assembled chromonics ͓11͔, fd virus ͓12͔, f-actin ͓13͔, and vanadium pentoxide ͓14,15͔. These droplets have in common their unusual elongated, spindlelike shape. This shape can be explained by the preferential planar anchoring of the nematic director at the interface with the isotropic phase. The competition between surface tension and the elastic deformation of the bipolar director field that accommodates this preferential planar anchoring plausibly determines the optimal aspect ratio ͑Fig. 1͒. If the director field of a tactoid is indeed bipolar with field lines connecting two boojum surface defects, then its shape, as described, e.g., by the aspect ratio or the tip angle, depends on its physical dimensions because the surface and bulk elastic energies scale differently with drop...
Liquid crystal ordering is an opportunity to develop novel materials and applications with carbon nanotubes spontaneously aligned on macroscopic scales. Nevertheless, achievement of large orientational order parameter and extended monodomains remains challenging. In this work, we show that shortening nanotubes allows the formation of liquid crystals that can easily be oriented under the form of large macroscopic monodomains. The orientational order parameter of single-wall nanotube liquid crystals measured by polarized Raman spectroscopy at the isotropic−nematic transition exceeds by far the value reported in previous experiments. The presently measured order parameter approaches the value theoretically expected for liquid crystals made of rigid rods in solution. This finding suggests that the production of highly ordered nanotube-based liquid crystals was presumably limited in earlier contributions by the length and waviness of long nanotubes. Both factors increase the material viscosity, can yield some elasticity, and stabilize topological defects.
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