Dynamics of crystal structure formation in spincoated colloidal films

The spin-coating of colloidal suspensions is an inherently nonequilibrium process that gives rise to highly reproducible, but polycrystalline, films with different symmetries depending on experimental parameters. In this study, we explore the transient dynamics of evaporative colloid spin-coating for the first time, via a combination of high-speed imaging, atomic force microscopy, static photography, and scanning electron microscopy. As the wet colloidal film thins and dries, we observe several symmetry transitions, while at the same time remarkably, the thinning rate (in nondimensional time units) collapses to one universal curve for all rotation rates. We correlate static and dynamic measures of crossovers in ordering regimes, and obtain an estimate of the evaporation rate in the late stage of drying. We conclude that the thinning dynamics controls the local volume fraction and stress profiles, which in turn drives the structural transitions

Quantifying disorder in colloidal films spin-coated onto patterned substrates

Polycrystals of thin colloidal deposits, with thickness controlled by spin-coating speed, exhibit axial symmetry with local 4-fold and 6-fold symmetric structures, termed orientationally correlated polycrystals (OCPs). While spin-coating is a very facile technique for producing large-area colloidal deposits, the axial symmetry prevents us from achieving true long-range order. To obtain true long-range order, we break this axial symmetry by introducing a patterned surface topography and thus eliminate the OCP character. We then examine symmetry- independent methods to quantify order in these disordered colloidal deposits. We find that all the information in the bond-orientational order parameters is well captured by persistent homology analysis methods that only use the centers of the particles as input data. It is expected that these methods will prove useful in characterizing other disordered structures

Dynamics of crystal structure formation in spincoated colloidal films

The spin-coating of colloidal suspensions is an inherently nonequilibrium process that gives rise to highly reproducible, but polycrystalline, films with different symmetries depending on experimental parameters. In this study, we explore the transient dynamics of evaporative colloid spin-coating for the first time, via a combination of high-speed imaging, atomic force microscopy, static photography, and scanning electron microscopy. As the wet colloidal film thins and dries, we observe several symmetry transitions, while at the same time remarkably, the thinning rate (in nondimensional time units) collapses to one universal curve for all rotation rates. We correlate static and dynamic measures of crossovers in ordering regimes, and obtain an estimate of the evaporation rate in the late stage of drying. We conclude that the thinning dynamics controls the local volume fraction and stress profiles, which in turn drives the structural transitions

Dynamics, crystallization, and structures in colloid spin coating

Spin coating is an out-of-equilibrium technique for producing polymer films and colloidal crystals quickly and reproducibly. In this review, we present an overview of theoretical and experimental studies of the spin coating of colloidal suspensions. The dynamics of the spin coating process is discussed first, and we present insights from both theory and experiment. A key difference between spin coating with polymer solutions and with monodisperse colloidal suspensions is the emergence of long range (centimeter scale) orientational correlations in the latter. We discuss experiments in different physical regimes that shed light on the many unusual partially ordered structures that have long-range orientational order, but no long-range translational order. The nature of these structures can be tailored by adding electric or magnetic fields during the spin coating procedure. These partially ordered structures can be considered as model systems for studying the fundamentals of poorly crystalline and defect-rich solids, and they can also serve as templates for patterned and/or porous optical and magnetic materials

Orientationally correlated colloidal polycrystals without long-range positional order

We probe the local and global structure of spin-coated colloidal crystals via laser diffraction measurements and scanning electron and atomic force microscopies, and find that they are unique three-dimensional orientationally correlated polycrystals, exhibiting short-range positional order but long-range radial orientational correlations, reminiscent of—but distinct from—two-dimensional colloidal hexatic phases. Thickness and symmetries are controllable by solvent choice and spin speed. While the polycrystallinity of these colloidal films limits their applicability to photonics, we demonstrate their feasibility as templates to make crack-free magnetic patterns