A surface having a spatial gradient in its surface free energy was capable of causing drops of water placed on it to move uphill. This motion was the result of an imbalance in the forces due to surface tension acting on the liquid-solid contact line on the two opposite sides ("uphill" or "downhill") of the drop. The required gradient in surface free energy was generated on the surface of a polished silicon wafer by exposing it to the diffusing front of a vapor of decyltrichlorosilane, Cl(3)Si(CH(2))(9)CH(3). The resulting surface displayed a gradient of hydrophobicity (with the contact angle of water changing from 97 degrees to 25 degrees ) over a distance of 1 centimeter. When the wafer was tilted from the horizontal plane by 15 degrees , with the hydrophobic end lower than the hydrophilic, and a drop of water (1 to 2 microliters) was placed at the hydrophobic end, the drop moved toward the hydrophilic end with an average velocity of approximately 1 to 2 millimeters per second. In order for the drop to move, the hysteresis in contact angle on the surface had to be low (=10 degrees ).
It is demonstrated that, while the Lifshitz-van der Waals (ylw) and the polar, Lewis acid-base ( ) surface tension components are additive, the Lewis acid-base electron-acceptor ( +) and electron-donor ( ~) surface tension parameters (which on account of the intrinsic asymmetry of their interactions are connected in a more complex manner) are not additive. Contact angle data cannot, in general, be correlated with a single surface tension property. The relation between contact angles and the three controlling parameters YgW, 7s> and § of a polar solid, S, cannot be established by means of one single equation. These three unknowns can, however, be determined by means of contact angle measurements with three different liquids L (of which two must be polar and H-bonding), which are completely characterized as to their respective ylW, Yl, and £ parameters by using a modified Young-Good-Girifalco-Fowkes equation 3 times.In view of these considerations, recent claims to have proven the applicability of a single "equation of state" are shown to be spurious. angle on a particular solid would be found to have the same surface tension. Table I shows that this is not the case. Water and glycerol form nearly the same contact angle on four of the solids. But the surface tensions of the two liquids differ by 12%, and the contact angles of the two liquids are significantly different on six other solids.Further, while glycerol spreads on flat surfaces of a gel encasing water (which could be expected), it is a curious finding that water also spreads on flat surfaces of a gel encasing glycerol (see Table II). It is not possible to explain this result by means of the equation of state.
The movement of liquid drops on a surface with a radial surface tension gradient is described here. When saturated steam passes over a colder hydrophobic substrate, numerous water droplets nucleate and grow by coalescence with the surrounding drops. The merging droplets exhibit two-dimensional random motion somewhat like the Brownian movements of colloidal particles. When a surface tension gradient is designed into the substrate surface, the random movements of droplets are biased toward the more wettable side of the surface. Powered by the energies of coalescence and collimated by the forces of the chemical gradient, small drops (0.1 to 0.3 millimeter) display speeds that are hundreds to thousands of times faster than those of typical Marangoni flows. This effect has implications for passively enhancing heat transfer in heat exchangers and heat pipes.
Following the development of a methodology for determining the apolar components as well as the electron donor and the electron acceptor parameters of the surface tension of polar surfaces, surfaces of a number of quite common materials were found to manifest virtually only electron donor properties and no, or hardly, any electron acceptor properties. Such materials may be called monopolar; they can strongly interact with bipolar materials (e.g., with polar liquids such as water); but one single polar parameter of a monopolar material cannot contribute to its energy of cohesion. Monopolar materials manifesting only electron acceptor properties also may exist, but they do not appear to occur in as great an abundance. Among the electron donor monopolar materials are: polymethylmethacrylate, polyvinylalcohol, polyethyleneglycol, proteins, many polysaccharides, phospholipids, nonionic surfactants, cellulose esters, etc. Strongly monopolar materials of the same sign repel each other when immersed or dissolved in water or other polar liquids. The interfacial tension between strongly monopolar surfaces and water has a negative value. This leads to a tendency for water to penetrate between facing surfaces of a monopolar substance and hence, to repulsion between the molecules or particles of such a monopolar material, when immersed in water, and thus to pronounced solubility or dispersibility. Monopolar repulsion energies can far outweigh Lifshitz-van der Waals attractions as well as electrostatic and "steric" repulsions. In aqueous systems the commonly observed stabilization effects, which usually are ascribed to "steric" stabilization, may in many instances be attributed to monopolar repulsion between nonionic stabilizing molecules. The repulsion between monopolar molecules of the same sign can also lead to phase separation in aqueous solutions (or suspensions), where not only two, but multiple phases are possible. Negative interfacial tensions between monopolar surfactants and the brine phase can be the driving force for the formation of microemulsions; such negative interfacial tensions ultimately decay and stabilize at a value very close to zero. Strongly monopolar macromolecules or particles surrounded by oriented water molecules of hydration can still repel each other, albeit to an attenuated degree. This repulsion was earlier perceived as caused by "hydration pressure". A few of the relevant colloid and surface phenomena are reviewed and re-examined in the light of the influence of surface monopolarity on these phenomena.
Our understanding of the "long range" electrodynamic, electrostatic, and polar interactions that dominate the organization of small objects at separations beyond an interatomic bond length is reviewed. From this basic-forces perspective, a large number of systems are described from which one can learn about these organizing forces and how to modulate them. The many practical systems that harness these nanoscale forces are then surveyed. The survey reveals not only the promise of new devices and materials, but also the possibility of designing them more effectively.
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