Grain splitting is a mechanism for grain coarsening in colloidal polycrystals.

In established theories of grain coarsening, grains disappear either by shrinking or by rotating as a rigid object to coalesce with an adjacent grain. Here we report a third mechanism for grain coarsening, in which a grain splits apart into two regions that rotate in opposite directions to match two adjacent grains' orientations. We experimentally observe both conventional grain rotation and grain splitting in two-dimensional colloidal polycrystals. We find that grain splitting occurs via independently rotating "granules" whose shapes are determined by the underlying triangular lattices of the two merging crystal grains. These granules are so small that existing continuum theories of grain boundary energy are inapplicable, so we introduce a hard sphere model for the free energy of a colloidal polycrystal. We find that, during splitting, the system overcomes a free energy barrier before ultimately reaching a lower free energy when splitting is complete. Using simulated splitting events and a simple scaling prediction, we find that the barrier to grain splitting decreases as grain size decreases. Consequently, grain splitting is likely to play an important role in polycrystals with small grains. This discovery suggests that mesoscale models of grain coarsening may offer better predictions in the nanocrystalline regime by including grain splitting.

Local Melting Attracts Grain Boundaries in Colloidal Polycrystals.

We find that laser-induced local melting attracts and deforms grain boundaries in 2D colloidal crystals. When a melted region in contact with the edge of a crystal grain recrystallizes, it deforms the grain boundary-this attraction is driven by the multiplicity of deformed grain boundary configurations. Furthermore, the attraction provides a method to fabricate artificial colloidal crystal grains of arbitrary shape, enabling new experimental studies of grain boundary dynamics and ultimately hinting at a novel approach for fabricating materials with designer microstructures.

Entropy-driven crystal formation on highly strained substrates.

In heteroepitaxy, lattice mismatch between the deposited material and the underlying surface strongly affects nucleation and growth processes. The effect of mismatch is well studied in atoms with growth kinetics typically dominated by bond formation with interaction lengths on the order of one lattice spacing. In contrast, less is understood about how mismatch affects crystallization of larger particles, such as globular proteins and nanoparticles, where interparticle interaction energies are often comparable to thermal fluctuations and are short ranged, extending only a fraction of the particle size. Here, using colloidal experiments and simulations, we find particles with short-range attractive interactions form crystals on isotropically strained lattices with spacings significantly larger than the interaction length scale. By measuring the free-energy cost of dimer formation on monolayers of increasing uniaxial strain, we show the underlying mismatched substrate mediates an entropy-driven attractive interaction extending well beyond the interaction length scale. Remarkably, because this interaction arises from thermal fluctuations, lowering temperature causes such substrate-mediated attractive crystals to dissolve. Such counterintuitive results underscore the crucial role of entropy in heteroepitaxy in this technologically important regime. Ultimately, this entropic component of lattice mismatched crystal growth could be used to develop unique methods for heterogeneous nucleation and growth of single crystals for applications ranging from protein crystallization to controlling the assembly of nanoparticles into ordered, functional superstructures. In particular, the construction of substrates with spatially modulated strain profiles would exploit this effect to direct self-assembly, whereby nucleation sites and resulting crystal morphology can be controlled directly through modifications of the substrate.

How the cucumber tendril coils and overwinds.

The helical coiling of plant tendrils has fascinated scientists for centuries, yet the underlying mechanism remains elusive. Moreover, despite Darwin's widely accepted interpretation of coiled tendrils as soft springs, their mechanical behavior remains unknown. Our experiments on cucumber tendrils demonstrate that tendril coiling occurs via asymmetric contraction of an internal fiber ribbon of specialized cells. Under tension, both extracted fiber ribbons and old tendrils exhibit twistless overwinding rather than unwinding, with an initially soft response followed by strong strain-stiffening at large extensions. We explain this behavior using physical models of prestrained rubber strips, geometric arguments, and mathematical models of elastic filaments. Collectively, our study illuminates the origin of tendril coiling, quantifies Darwin's original proposal, and suggests designs for biomimetic twistless springs with tunable mechanical responses.

3D imaging and mechanical modeling of helical buckling in Medicago truncatula plant roots.

We study the primary root growth of wild-type Medicago truncatula plants in heterogeneous environments using 3D time-lapse imaging. The growth medium is a transparent hydrogel consisting of a stiff lower layer and a compliant upper layer. We find that the roots deform into a helical shape just above the gel layer interface before penetrating into the lower layer. This geometry is interpreted as a combination of growth-induced mechanical buckling modulated by the growth medium and a simultaneous twisting near the root tip. We study the helical morphology as the modulus of the upper gel layer is varied and demonstrate that the size of the deformation varies with gel stiffness as expected by a mathematical model based on the theory of buckled rods. Moreover, we show that plant-to-plant variations can be accounted for by biomechanically plausible values of the model parameters.

Evolution of spur-length diversity in Aquilegia petals is achieved solely through cell-shape anisotropy.

The role of petal spurs and specialized pollinator interactions has been studied since Darwin. Aquilegia petal spurs exhibit striking size and shape diversity, correlated with specialized pollinators ranging from bees to hawkmoths in a textbook example of adaptive radiation. Despite the evolutionary significance of spur length, remarkably little is known about Aquilegia spur morphogenesis and its evolution. Using experimental measurements, both at tissue and cellular levels, combined with numerical modelling, we have investigated the relative roles of cell divisions and cell shape in determining the morphology of the Aquilegia petal spur. Contrary to decades-old hypotheses implicating a discrete meristematic zone as the driver of spur growth, we find that Aquilegia petal spurs develop via anisotropic cell expansion. Furthermore, changes in cell anisotropy account for 99 per cent of the spur-length variation in the genus, suggesting that the true evolutionary innovation underlying the rapid radiation of Aquilegia was the mechanism of tuning cell shape.

Glassy dislocation dynamics in 2D colloidal dimer crystals.

Although glassy relaxation is typically associated with disorder, here we report on a new type of glassy dynamics relating to dislocations within 2D crystals of colloidal dimers. Previous studies have demonstrated that dislocation motion in dimer crystals is restricted by certain particle orientations. Here, we drag an optically trapped particle through such dimer crystals, creating dislocations. We find a two-stage relaxation response where initially dislocations glide until encountering particles that cage their motion. Subsequent relaxation occurs logarithmically slowly through a second process where dislocations hop between caged configurations. Finally, in simulations of sheared dimer crystals, the dislocation mean squared displacement displays a caging plateau typical of glassy dynamics. Together, these results reveal a novel glassy system within a colloidal crystal.

Direct measurements of island growth and step-edge barriers in colloidal epitaxy.

Epitaxial growth, a bottom-up self-assembly process for creating surface nano- and microstructures, has been extensively studied in the context of atoms. This process, however, is also a promising route to self-assembly of nanometer- and micrometer-scale particles into microstructures that have numerous technological applications. To determine whether atomic epitaxial growth laws are applicable to the epitaxy of larger particles with attractive interactions, we investigated the nucleation and growth dynamics of colloidal crystal films with single-particle resolution. We show quantitatively that colloidal epitaxy obeys the same two-dimensional island nucleation and growth laws that govern atomic epitaxy. However, we found that in colloidal epitaxy, step-edge and corner barriers that are responsible for film morphology have a diffusive origin. This diffusive mechanism suggests new routes toward controlling film morphology during epitaxy.

Dislocations and vacancies in two-dimensional mixed crystals of spheres and dimers.

In colloidal crystals of spheres, dislocation motion is unrestricted. On the other hand, recent studies of relaxation in crystals of colloidal dimer particles have demonstrated that the dislocation dynamics in such crystals are reminiscent of glassy systems. The observed glassy dynamics arise as a result of dislocation cages formed by certain dimer orientations. In the current study, we use experiments and simulations to investigate the transition that arises when a pure sphere crystal is doped with an increasing concentration of dimers. Specifically, we focus on both dislocation caging and vacancy motion. Interestingly, we find that any nonzero fraction of dimers introduces finite dislocation cages, suggesting that glassy dynamics are present for any mixed crystal. However, we have also identified a vacancy-mediated uncaging mechanism for releasing dislocations from their cages. This mechanism is dependent on vacancy diffusion, which slows by orders of magnitude as the dimer concentration is increased. We propose that in mixed crystals with low dimer concentrations vacancy diffusion is fast enough to uncage dislocations and delay the onset of glassy dislocation dynamics.

Restricted dislocation motion in crystals of colloidal dimer particles.

At high area fractions, monolayers of colloidal dimer particles form a degenerate crystal (DC) structure in which the particle lobes occupy triangular lattice sites while the particles are oriented randomly along any of the three lattice directions. We report that dislocation glide in DCs is blocked by certain particle orientations. The mean number of lattice constants between such obstacles is Z[over](exp)=4.6+/-0.2 in experimentally observed DC grains and Z[over](sim)=6.18+/-0.01 in simulated monocrystalline DCs. Dislocation propagation beyond these obstacles is observed to proceed through dislocation reactions. We estimate that the energetic cost of dislocation pair separation via such reactions in an otherwise defect free DC grows linearly with final separation, hinting that the material properties of DCs may be dramatically different from those of 2-D crystals of spheres.