Cyanine dyes are widely used in studies of various molecularly organized and biological systems [1][2][3][4]. Examples of such organized systems are microemulsions, normal and reverse micelles, lipid vesicles, and others. In these systems, individual stages of photosynthesis are modeled, and supramolecular systems for solar energy conversion are designed [3]. The formation of J aggregates in vesicles was observed in [5], when positively charged dye molecules were adsorbed on the negatively charged vesicle interface. In this case, strong Coulomb interaction between dye molecules and the vesicle interface can lead to the formation of J aggregates only at a very high concentration of dye molecules, and the minimum number of dye molecules necessary for J aggregate formation is 60 [6]. It has been shown that dye molecules are preferentially localized in the vesicles that already contain dye molecules rather than are uniformly distributed among all vesicles [3].The behavior of cyanines in solutions was intensely studied in the presence of surfactants [7][8][9], in normal [10-12] and reverse micelles [8,9,13]. It has been shown on the basis of spectral data that the decomposition of the dimer and the conversion of the cis-monomer to the trans -isomer occurs in reverse AOT micelles [14]. This cis -trans isomerization is due to strong electrostatic interaction of the dye with hydrophilic AOT groups at the interface between the organic phase and water, whereas the isomerization effect is much weaker in reverse micelles of neutral Triton X-100. Electrostatic interaction results in polarization and alignment of charged subunits in the dye molecule along the electric field, leading to conversion of the cis -to the transisomer. Hence, the absence of dye dimers in reverse micelles, as noted in [14], is due to the fact that the trans -isomer, unlike the cis -isomer, does not tend to form dimers in an aqueous medium.The preparation of monodispersed J aggregates of a given size, including those of an extremely small size, is a fundamental problem of great practical importance.One of possible ways of its solving seems to be the use of reverse micelles.Information on possible aggregated states of cyanine dyes in reverse micelles is rather controversial. For example, it has been established [13] that one dye molecule at the most can be present in the water pool of a single micelle, and the probability of occurrence of two dye molecules is of the order of 10 -5 . On the other hand, it is stated [14,15] that in water pools of reverse micelles with W ≥ 5 ( W = [H 2 O]/[AOT]), dye J aggregates are formed even at average dye concentrations much lower than one dye molecule per micelle. Zhang and Liu [13] believe that a dye molecule in micelles with a small water-pool radius is compressed by the surfactant shell, which results in distortion of planarity of the molecule, and molecule transforms into the nonfluorescent twisted monomeric state. In micelles of a greater size, the dye molecule exists in the planar fluorescent state in the water ...