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1. Anisotropic particle multiphase equilibria in nonuniform fields

   https://doi.org/10.1063/5.0169659  

   Baron, Philippe B.; Hendley, Rachel S.; Bevan, Michael A. (September 2023, The Journal of Chemical Physics)

   We report a method to predict equilibrium concentration profiles of hard ellipses in nonuniform fields, including multiphase equilibria of fluid, nematic, and crystal phases. Our model is based on a balance of osmotic pressure and field mediated forces by employing the local density approximation. Implementation of this model requires development of accurate equations of state for each phase as a function of hard ellipse aspect ratio in the range k = 1–9. The predicted density profiles display overall good agreement with Monte Carlo simulations for hard ellipse aspect ratios k = 2, 4, and 6 in gravitational and electric fields with fluid–nematic, fluid–crystal, and fluid–nematic–crystal multiphase equilibria. The profiles of local order parameters for positional and orientational order display good agreement with values expected for bulk homogeneous hard ellipses in the same density ranges. Small discrepancies between predictions and simulations are observed at crystal–nematic and crystal–fluid interfaces due to limitations of the local density approximation, finite system sizes, and uniform periodic boundary conditions. The ability of the model to capture multiphase equilibria of hard ellipses in nonuniform fields as a function of particle aspect ratio provides a basis to control anisotropic particle microstructure on interfacial energy landscapes in diverse materials and applications. 

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2. Design rules for 2D field mediated assembly of different shaped colloids into diverse microstructures

   https://doi.org/10.1039/D2SM01078J  

   Hendley, Rachel S.; Zhang, Lechuan; Bevan, Michael A. (December 2022, Soft Matter)

   Assembling different shaped particles into ordered microstructures is an open challenge in creating multifunctional particle-based materials and devices. Here, we report the two-dimensional (2D) AC electric field mediated assembly of different shaped colloidal particles into amorphous, liquid crystalline, and crystalline microstructures. Particle shapes investigated include disks, ellipses, squares, and rectangles, which show how systematic variations in anisotropy and corner curvature determine the number and type of resulting microstructures. AC electric fields induce dipolar interactions to control particle positional and orientational order. Microstructural states are determined via particle tracking to compute order parameters, which agree with computer simulations and show how particle packing and dipolar interactions together produce each structure. Results demonstrate how choice of particle shape and field conditions enable kinetically viable routes to assemble nematic, tetratic, and smectic liquid crystal structures as well as crystals with stretched 4- and 6-fold symmetry. Results show it is possible to assemble all corresponding hard particle phases, but also show how dipolar interactions influence and produce additional microstructures. Our findings provide design rules for the assembly of diverse microstructures of different shaped particles in AC electric fields, which could enable scalable and reconfigurable particle-based materials, displays, and printing technologies. 

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3. Deposition and alignment of fiber suspensions by dip coating

   https://doi.org/10.1016/j.jcis.2023.06.180  

   Jeong, Deok-Hoon; Xing, Langqi; Lee, Michael Ka; Vani, Nathan; Sauret, Alban (November 2023, Journal of Colloid and Interface Science)

   Hypothesis: The dip coating of suspensions made of monodisperse non-Brownian spherical particles dispersed in a Newtonian fluid leads to different coating regimes depending on the ratio of the particle diameter to the thickness of the film entrained on the substrate. In particular, dilute particles dispersed in the liquid are entrained only above a threshold value of film thickness. In the case of anisotropic particles, in particular fibers, the smallest characteristic dimension will control the entrainment of the particle. Furthermore, it is possible to control the orientation of the anisotropic particles depending on the substrate geometry. In the thick film regime, the Landau-Levich-Derjaguin model remains valid if one account for the change in viscosity. Experiment: To test the hypotheses, we performed dip-coating experiments with dilute suspensions of non-Brownian fibers with different length-to-diameter aspect ratios. We characterize the number of fibers entrained on the surface of the substrate as a function of the withdrawal velocity, allowing us to estimate a threshold capillary number below which all the particles remain in the liquid bath. Besides, we measure the angular distribution of the entrained fibers for two different substrate geometries: flat plates and cylindrical rods. We then measure the film thickness for more concentrated fiber suspensions. Findings: The entrainment of the fibers on a flat plate and a cylindrical rod is primarily controlled by the smaller characteristic length of the fibers: their diameter. At first order, the entrainment threshold scales similarly to that of spherical particles. The length of the fibers only appears to have a minor influence on the entrainment threshold. No preferential alignment is observed for non-Brownian fibers on a flat plate, except for very thin films, whereas the fibers tend to align themselves along the axis of a cylindrical rod for a large enough ratio of the fiber length to the radius of the cylindrical rod. The Landau-Levich-Derjaguin law is recovered for more concentrated suspension by introducing an effective capillary number accounting for the change in viscosity. 

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4. Disorder and demixing in bidisperse particle systems assembling bcc crystals

   https://doi.org/10.1063/5.0219037  

   Kennard, Jasmin J; Zelaya_Solano, H Jonathan; Biddulph, Caleb D; Prager, Ryan C; Dshemuchadse, Julia (August 2024, The Journal of Chemical Physics)

   Colloidal and nanoparticle self-assembly enables the creation of ordered structures with a variety of electronic and photonic functionalities. The outcomes of the self-assembly processes used to synthesize such structures, however, strongly depend on the uniformity of the individual nanoparticles. Here, we explore the simplest form of particle size dispersity—bidispersity—and its impact on the self-assembly process. We investigate the robustness of self-assembling bcc-type crystals via isotropic interaction potentials in binary systems with increasingly disparate particle sizes by determining their terminal size ratio—the most extreme size ratio at which a mixed binary bcc crystal forms. Our findings show that two-well pair potentials produce bcc crystals that are more robust with respect to particle size ratio than one-well pair potentials. This suggests that an improved self-assembly process is accomplished with a second attractive length scale encoded in the particle–particle interaction, which stabilizes the second-nearest neighbor shell. In addition, we document qualitative differences in the process of ordering and disordering: in bidisperse systems of particles interacting via one-well potentials, we observe a breakdown of order prior to demixing, while in systems interacting via two-well potentials, demixing occurs first and bcc continues to form in parts of the droplet down to low size ratios. 

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5. High-Density and Well-Aligned Hierarchical Structures of Colloids Assembled under Orthogonal Magnetic and Electric Fields

   https://doi.org/10.1021/acsnano.4c11957  

   Haque, Md Ashraful; Maestas, Joseph R; Zhu, Xingrui; Hanson, Benjamin L; Wu, David T; Wu, Ning (January 2025, ACS Nano)

   Colloids can be used either as model systems for directed assembly or as the necessary building blocks for making functional materials. Previous work primarily focused on assembling colloids under a single external field, where controlling particle−particle interactions is limited. This work presents results under a combination of electric and magnetic fields. When these two fields are orthogonally applied, we can independently tune the magnitude and direction of the dipolar attraction and repulsion between the particles. As a result, we obtain well-aligned, highly dense, but individually separated linear chains at intermediate particle concentrations. Both the inter- and intrachain spacings can be tuned by adjusting the particle concentration and relative strengths of both fields. At high particle concentrations and by tuning the electric field frequency, the individual microspheres can assemble into colloidal oligomers such as trimers, tetramers, heptamers, and nonamers in response to the electric field due to the synergy between dipolar and electrohydrodynamic interactions. These oligomers, in turn, serve as building blocks for making hierarchical structures with finer architectures upon superimposing a one-dimensional (1D) magnetic field. In addition to experiments, Monte Carlo (MC) simulations have been performed on colloids confined near the electrode, interacting through a Stockmayer-like potential. They faithfully reproduce key observations in the experiments. Our work demonstrates the potential of using orthogonal electric and magnetic fields to assemble diversified types of highly aligned structures for applications in high-strength composites, optical materials, or structured battery electrodes. 

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