Second harmonic generation (SHG) and sum frequency generation (SFG) techniques have been used to probe L/L interfaces and have the potential to provide interface dynamic properties. 5,11,16 Neutron specular reflectivity measurements have been used to study the effect of surfactants on the roughness of L/L interfaces. 6 Many researchers have investigated liquid surfaces by measuring capillary waves. [23][24][25][26][27][28][29][30][31] Since capillary waves reflect the fundamental properties of the surface or interfacial region, much effort has been made to observe them and to analyze their spectra. The theoretical understanding of these waves is well estimated in hydrodynamics, and light scattering from the waves is also widely used to monitor the L/L interfaces.2 In our previous papers, 13,21,22 we reported that a developed timeresolved quasi-elastic laser-scattering (QELS) method was a powerful tool for studying molecular dynamics at L/L interfaces. The QELS method monitors the change of the frequencies of the capillary waves, which are spontaneously generated by thermal fluctuation at L/L interfaces. The QELS method has good interface selectivity for overcoming the problem of interference by bulk phases, because the capillary wave is a characteristic phenomenon at the interface.Chemical processes, such as formation of monolayers or transformation of chemical species at the interface, cause changes of Gibbs free energy there. 32,33 In turn, these Gibbs free energy changes cause changes of interfacial tension. So it has been assumed that these chemical processes can be monitored by observing changes of interfacial tension. As we described previously, 13,21 the capillary wave frequency is a function of interfacial tension and the change in the interfacial tension depends on the change in the number density of surfactant molecules at the interface; then the QELS method allows observation of the dynamic change of L/L interfaces such as the formation of a lipid monolayer, 13 or the adsorption of surfactant molecules. 21,22 Compared with conventional interfacial tension measurements, the QELS method has the obvious advantage of being able to probe interfaces between two bulk phases without any mechanical perturbation.It is suitable for in situ monitoring of interfaces. Furthermore, owing to its improved time resolution, each power spectrum can be obtained in 1 ms to 1 s, so the method can be used to monitor the dynamic change in number density of surfactants at L/L interfaces in a real environment. The simplicity of the measurement is also an advantage.Using the QELS method, we have successfully monitored the dynamic and collective behavior of three kinds of surfactant molecules with different charges at the water/nitrobenzene (W/NB) interface, and found that the behavior of these molecules differs from each other. 21,22 Particularly for anionic sodium dodecyl sulfate (SDS) molecules, when the injected concentration is above the critical micelle concentration (cmc), the relative number density decreases with an incr...