Surface coatings and patterning technologies are essential for various physicochemical applications. In this Letter, we describe key parameters to achieve uniform particle coatings from binary solutions: First, multiple sequential Marangoni flows, set by solute and surfactant simultaneously, prevent non-uniform particle distributions and continuously mix suspended materials during droplet evaporation. Second, we show the importance of particle-surface interactions that can be established by surface-adsorbed macromolecules. To achieve a uniform deposit in a binary mixture, a small concentration of surfactant and surface-adsorbed polymer (0.05 wt% each) is sufficient, which offers a new physicochemical avenue for control of coatings.
PACS numbers:An evaporating liquid drop, either single or multicomponent, containing solutes or particulates leaves a deposit whose form is determined by various parameters, for instance internal flow fields [1][2][3], liquid compositions [4][5][6][7][8][9][10], and interactions between suspended particles and a solid substrate [11][12][13][14], which are crucial for coating processes. In particular, control of the deposit uniformity and thickness can be important in surface patterning [15][16][17], ink-jet [4,18,19] and 3D printing technologies [20]. These processes are complex because of physicochemical dynamics that arise from Marangoni effects [2, 5-10, 12, 21, 22] and particle deposition mechanisms [11,12,14,23]. In fact, although a binary mixture is used quite often to achieve uniform particle deposition from droplets smaller than 100 µm [4,18,19], to our best knowledge such coatings have not been achieved for larger droplets. Furthermore, while the wetting and dewetting behaviors of binary mixture drops have been investigated [24,25], the relation between the deposition pattern and the evaporatively driven flow field in a binary mixture droplet is incomplete (Table S1, Supporting Information (SI)) [26].In this Letter, to achieve a uniform coating, we identify key characteristics of a multicomponent solution, which consists of a binary mixture, surface-active surfactant, and surface-adsorbed polymer. We were motivated to pursue the ideas here from examining a whisky droplet after drying on an ordinary glass where it creates a relatively uniform particle deposit (see Fig. 1), which is in contrast to the well-known 'coffee-ring stain' [1]. Based on our understanding of the drying and coating mechanisms of binary liquid droplets, whisky droplets, and more complex solution droplets, we design a model liquid that yields nearly uniform deposits by taking the approach that whisky is an ethanol-water mixture containing diverse dissolved molecules, which contribute to the * Electronic address: hastone@princeton.edu complexity of the system, the flows, and the final particle deposits.We begin with a few remarks about whisky, since it serves as a model complex mixture, where nearly uniform particle deposits are observed after drying. Whisky is an alcoholic liquid (ethanol:water, 35:65 % b...