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COMMUNICATIONsubwavelength imaging (superlens). [ 12,13 ] In addition, doping sphere-based photonic crystals with rare earths, lanthanides, organic dyes and quantum dots has established properties such as suppression or enhancement of spontaneous emission and photonic crystal lasing due to multiple refl ections and high density of states at the photonic band gap edges. [14][15][16] Only a handful of experimental reports address uniform nonspherical colloidal building blocks (i.e., size range between 400 nm and 1.5 micrometers for photonic crystals in the visible and nearinfrared regimes) with an active optical functionality (i.e., luminescence) at the single particle level.The present work develops fullerene microcrystals as a new materials platform, suitable for 'active' light emitting elements in colloid-based photonic crystals. The materials support singlet excited states that tend to be self-trapped by localized lattice deformation (i.e., Jahn-Teller distortion) and recombine to produce a characteristic red photoluminescence (PL). [17][18][19][20] These high refractive index and transparent building blocks (λ > 560 nm) may also support photonic band gaps in direct structures as compared to the common silica and polymer sphere-based structures which must be backfi lled with semiconductors such as Si and GaAs. [ 11 ] Fullerene molecular crystals have previously been synthesized in a variety of bulk to mesoscale forms including thick and thin fi lms, [ 21 ] wire arrays, [ 22 ] whiskers [ 23 ] and platelets. [ 24 ] Micrometer and sub-micrometer crystals have also been prepared with anisotropic morphology using solution-based techniques such as precipitation at the interface between immiscible liquids (LLIP, liquid-liquid interfacial precipitation), [24][25][26] and evaporation-assisted growth from drops on a substrate. [27][28][29][30] Control of size and shape dispersity with these methods is still lacking. In contrast, microcrystal growth in emulsifi ed solvent-nonsolvent mixtures (co-solvent precipitation) has yielded colloidal particles with tunable shapes, crystal structure and monodispersity. [31][32][33][34] Droplet shrinkage over time in miscible liquids causes local supersaturation of the fullerenes and leads to particle nucleation. The solvent properties (i.e., molecular shape, fullerene solubility, dipole moment, miscibility, interdiffusion rate, etc.), solvent-antisolvent ratio, concentration, temperature and mixing conditions determine the colloidal chemistry and morphology. [31][32][33][34][35] For example, crystallization of C 60 with CS 2 in 2-propanol resulted in bipyramidal-shaped particles, C 70 crystallized with CS 2 in 1-propanol produced rugby ball shapes as well as rhombic dodecahedra, and C 70 with mesitylene in 2-propanol solution produced cubes. [ 31,32 ] Here, we report the synthesis of shape diverse and monodisperse microcrystal solvates using co-solvent precipitation with C 60 and C 70 fullerene-methylbenzene solutions in 2-propanol as a poor solvent. The photol...