The spontaneous spreading of a thin liquid film along the surface of a deep liquid layer of higher surface tension is a ubiquitous process which provides rapid and efficient surface transport of organic or biological material. For a source of constant concentration, the leading edge of a nonvolatile, immiscible film driven to spread by gradients in surface tension is known to advance as t 3/4 in time. Recent experiments using laser shadowgraphy to detect the advancing front of spreading films indicate, however, that immiscible but volatile sources of constant concentration spread with a reduced exponent according to t 1/2. Using a novel technique whereby fluorescent lines are inscribed in water, we have detected the evolution of a thermal instability beneath the leading edge of volatile films which strongly resembles a Rayleigh-Bénard roll. We propose that the increased dissipation from this rotational flow structure is likely responsible for the reduction in spreading exponent. This observation suggests a conceptual framework for coupling the effects of evaporation to the dynamics of spreading. © 1998 American Institute of Physics. ͓S1070-6631͑98͒01607-9͔
I. SPONTANEOUS SPREADING ON A DEEP LIQUID LAYERWhen a liquid substrate is contacted by a film of lower surface tension, surface traction is produced in proportion to the difference in surface tension between the liquid support and the spreading film. This traction creates rapid and spontaneous flow toward regions of higher surface tension. The speed of the spreading film is known to increase with the magnitude of the spreading coefficient defined by Sϭ␥ 1 Ϫ␥ 2 Ϫ␥ 12 , where ␥ 1 denotes the surface tension of the clean liquid support, ␥ 2 the surface tension of the spreading film, and ␥ 12 the interfacial tension between the spreading film and supporting liquid.1 This spreading coefficient is related to the local gradient in surface tension, ,xץ/␥ץ through the relation Sϭ͐ 0 L(t) xץ/␥ץ dx, where the coordinate x denotes the horizontal or radial direction of spreading and L(t) denotes the length of the surface active film at time t after contact with the liquid support. In the examples discussed below, the gradients in surface tension are caused by variations in the surface concentration, ⌫, of the spreading film where .)xץ/⌫ץ()⌫ץ/␥ץ(xϭץ/␥ץ The spontaneous advance of a surface film driven by this type of shear stress is called Marangoni driven spreading, 2 which occurs for positive values of the spreading coefficient. A small scale example of this spreading process occurs during the casting of Langmuir-Blodgett films. In the fabrication of these films, organic or biological molecules are dissolved in a solvent like hexane or carbon tetrachloride which spreads rapidly and spontaneously over the surface of water. The organic solvent, which has a lower surface tension than pure water, acts as the carrier liquid to transport molecules along the water surface under the action of Marangoni stresses. 3 The solvent film eventually evaporates leaving behin...