CdSe/ZnS quantum dots were chosen for their higher quantum yield and easier fluorescence microscopic visualization relative to uncoated CdSe quantum dots.) [29] Separate polymerization studies using catalyst 3 are in progress:K. Breitenkamp, T. Emrick, unpublished. Dynamic Self-Assembly of the Liquid-Crystalline Smectic A Phase** By S. Krishna Prasad,* Geetha G. Nair, and Gurumurthy HegdePhotonics, in which light can be controlled by light as a stimulus, is being proposed as the future technology for highspeed information processing. Liquid-crystalline systems are known for the large change in their optical effects as a response to even weak external fields, and are being considered for other optical applications apart from their phenomenal success in flat-panel devices. A niche area of research that is being actively pursued in this regard is the photoinduced phase transitions in liquid-crystalline systems and the concomitant changes in birefringence which are useful for optical devices. In all the cases reported to date, the photoinduced transition always leads to a phase that, in any case, exists in the thermal cycle. Here we report the first exception to such an established principle. The employed guest±host system containing photoactive azobenzene guest molecules does not exhibit the smectic A phase in the absence of UV radiation. However, the smectic A phase is induced and stabilized only in the presence of UV light. To explain this dynamic self-assembly into a layered phase from a simple orientationally ordered fluid phase, we propose an argument based on photoinduced nanophase segregation and a frustrated spin-gas model.Research on materials which exhibit photostimulated changes in their structural, optical, or electrical properties is being pursued aggressively.[1±3] Liquid crystals (LCs) as photoactive media have attracted significant attention in this regard owing to the combination of molecular motion [4] that could result from the action of light and the self-assembling nature of these structured fluids. On the other hand, phase segregation as a mechanism on different length scales plays a very important role in the formation of a variety of LC structures, even to the extent of being the basis of realizing certain LC phases. A more interesting aspect is the control of nanoscalelevel segregation by external means. Such a phenomenon has been observed, for example, in electrospun fibers containing carbon nanotubes, [5] in molecule-thick elastomers with interesting microtribological properties, [6] and in the appearance of chirality in achiral systems. [7] From a device-application point of view, the combination of self-assembly and phase segregation has been well exploited in optical shutters formed by polymer-dispersed LCs, [8] very high-charge-mobility devices with columnar LCs, [9] etc.An important interplay between light and the structure of LCs was first observed by Folks et al. [10] and has been excellently explained by the simulation studies of Lansac et al., [11] who introduced the concept ...