Biotropic liquid crystal phase transformations in cellulose-producing bacterial communities.

Biological functionality is often enabled by a fascinating variety of physical phenomena that emerge from orientational order of building blocks, a defining property of nematic liquid crystals that is also pervasive in nature. Out-of-equilibrium, "living" analogs of these technological materials are found in biological embodiments ranging from myelin sheath of neurons to extracellular matrices of bacterial biofilms and cuticles of beetles. However, physical underpinnings behind manifestations of orientational order in biological systems often remain unexplored. For example, while nematiclike birefringent domains of biofilms are found in many bacterial systems, the physics behind their formation is rarely known. Here, using cellulose-synthesizing Acetobacter xylinum bacteria, we reveal how biological activity leads to orientational ordering in fluid and gel analogs of these soft matter systems, both in water and on solid agar, with a topological defect found between the domains. Furthermore, the nutrient feeding direction plays a role like that of rubbing of confining surfaces in conventional liquid crystals, turning polydomain organization within the biofilms into a birefringent monocrystal-like order of both the extracellular matrix and the rod-like bacteria within it. We probe evolution of scalar orientational order parameters of cellulose nanofibers and bacteria associated with fluid-gel and isotropic-nematic transformations, showing how highly ordered active nematic fluids and gels evolve with time during biological-activity-driven, disorder-order transformation. With fluid and soft-gel nematics observed in a certain range of biological activity, this mesophase-exhibiting system is dubbed "biotropic," analogously to thermotropic nematics that exhibit solely orientational order within a temperature range, promising technological and fundamental-science applications.

Directing Liquid Crystalline Self-Organization of Rodlike Particles through Tunable Attractive Single Tips.

Dispersions of rodlike colloidal particles exhibit a plethora of liquid crystalline states, including nematic, smectic A, smectic B, and columnar phases. This phase behavior can be explained by presuming the predominance of hard-core volume exclusion between the particles. We show here how the self-organization of rodlike colloids can be controlled by introducing a weak and highly localized directional attractive interaction between one of the ends of the particles. This has been performed by functionalizing the tips of filamentous viruses by means of regioselectively grafting fluorescent dyes onto them, resulting in a hydrophobic patch whose attraction can be tuned by varying the number of bound dye molecules. We show, in agreement with our computer simulations, that increasing the single tip attraction stabilizes the smectic phase at the expense of the nematic phase, leaving all other liquid crystalline phases invariant. For a sufficiently strong tip attraction, the nematic state may be suppressed completely to get a direct isotropic liquid-to-smectic phase transition. Our findings provide insights into the rational design of building blocks for functional structures formed at low densities.

Elementary Edge and Screw Dislocations Visualized at the Lattice Periodicity Level in the Smectic Phase of Colloidal Rods.

Topological defects such as dislocations play a major role in science, from condensed matter and geophysics to cosmology. These line defects present in periodically ordered structures mediate phase transitions and determine many distinctive features of materials, from crystal growth to mechanical properties. However, despite theoretical predictions, the detailed structure of dislocations remains largely elusive. By using a model system of tip-labeled rod-shaped particles enabling improved resolution and contrast by optical microscopy, in situ visualization and quantitative characterization of elementary dislocations has been performed at the lattice periodicity level in a colloidal smectic phase. Thanks to the micrometer layer spacing, the displacement field around an edge dislocation has been experimentally established and compared with the profile predicted by elastic theory. The local morphology of screw dislocations has also been evidenced, with the determination of the core size as well as the chiral handedness of the defect. Self-diffusion experiments performed at the individual particle level reveal for the first time nematiclike or "melted" ordering of the defect core.

Rod-Like Virus-Based Multiarm Colloidal Molecules.

We report on the construction of multiarm colloidal molecules by tip-linking filamentous bacteriophages, functionalized either by biological engineering or chemical conjugation. The affinity for streptavidin of a genetically modified vector phage displaying Strep-tags fused to one end of the viral particle is measured by determining the dissociation constant, Kd. In order to improve both the colloidal stability and the efficiency of the self-assembly process, a biotinylation protocol having a chemical yield higher than 90% is presented to regioselectively functionalize the cystein residues located at one end of the bacteriophages. For both viral systems, a theoretical comparison is performed by developing a quantitative model of the self-assembly and interaction of the modified viruses with streptavidin compounds, which accurately accounts for our experimental results. Multiarm colloidal structures of different valencies are then produced by conjugation of these tip-functionalized viruses with streptavidin activated nanoparticles. We succeed to form stable virus-based colloidal molecules, whose number of arms, called valency, is solely controlled by tuning the molar excess. Thanks to a fluorescent labeling of the viral arms, the dynamics of such systems is also presented in real time by fluorescence microscopy.