In general, the transfer efficiency of the constructed two-step energy transfer was reduced to some extent (Table and). In a control experiment, free PBTB or Z1 without energy donors (K-1 or K-2) showed almost no fluorescence upon excitation, indicating efficient energy transfer from energy donor to acceptor (Figure ). Subsequently, the morphologies of the abovementioned individual molecules and ALHSs were investigated by scanning electron microscopy (SEM). The results showed that these nanoparticles appeared to be concave or almost regular spherical morphology (Figure and). Therefore, the sizes of the formed aggregates after assembly were further studied by dynamic light scattering (DLS) experiments. The results of DLS showed that spherical nanoparticles with larger average particle size were formed after the acceptors were mixed with donors (Figure and S18), indicating extensive interactions and coassembly processes between molecules. In addition, obvious Tyndall effects could be observed in all solutions (inset of Figure and S18), which also indicated that a large number of supramolecular nanoparticles were formed. White organic light-emitting materials are of significance because of their potential applications in light emitting devices and display media. Generally, white light emission can be achieved by a combination of the three primary (red, green, and blue) or two complementary colors (e.g. orange and blue) according to the Commission Internationale de L'Eclairage (CIE) chromaticity diagram. As the ratio of PBTB increased, the fluorescence color of the K-1/PBTB system changed from blue to orange (Figure ), indicating that white light emission can be realized by tuning the ratio of K-1 and PBTB. In contrast, it is speculated that the K-1/PBTB/Z1 system failed to achieve white light emission due to its color change from orange to red as the ratio of Z1 increased (Figure ). As expected, bright white light emission can be successfully realized with a CIE coordinate of (0.33, 0.34) at the ratio of K-1/PBTB = 200:1 (Figure and). When the energy donor was replaced by K-2, similar results were obtained in the corresponding ALHSs (Figure ). Due to the wide application of organophosphorus compounds in pharmaceuticals, pesticides, flame retardants, ligands and so on, relevant research reports are of great significance. Therefore, photocatalytic C-P bond formation has attracted great attention among chemists, especially the reports of ALHSs as photocatalysts. We then investigated the possibility of the above ALHSs and individual fluorescent dyes as photocatalysts in cross-dehydrogenative coupling (CDC) reactions, and optimized the conditions of photocatalytic C-P bond formation (Table and ). Entry Photocatalyst Solvent Yield (%) In a mixed solution of H2O-THF (19:1; v/v), benzothiazole 8a was selected as the model substrate for the reaction with diphenylphosphine oxide 9, and the effect of the photocatalysts was first investigated (Table ). The experiment results revealed that the target product 10a was formed in poor to moderate yields, when K-1, K-2, PBTB, and Z1 were employed as photocatalysts (Table , entries 1-4). The TLC analysis revealed that 8a was not fully transformed in all the above reactions. Notably, the reaction yield exhibited an impressive enhancement, reaching 87% when the K-1/PBTB ALHS was used as catalyst (Table , entry 5). Moreover, the solution emitted white light at the ratio of K-1/PBTB of 200:1. When the amount of catalyst was reduced to 3 mol%, the yield was slightly reduced (Table , entry 6). In addition, the improved equivalent of 9 failed to increase the yield, and the product 10a was obtained with a moderate yield of 65% (Table , entry 7). Subsequently, a series of control experiments were performed. As expected, trace amount of the product was observed in the N2 atmosphere (Table , entry 8), and a small amount of product (8%) was detected in the absence of photocatalysts (Table , entry 9). Unsurprisingly, this reaction did not occur in the absence of light (Table , entry 10). Since the maximum ΦET occurred when the K-1/PBTB was about 1000:40, the reaction was conducted under this ratio of donor/acceptor. The result showed that 72% yield of 10a can be obtained (Table , entry 11). For the same reason, the reaction was performed at the K-1/PBTB/Z1 ratio of 1000:40:14, and 10a was isolated in 70% yield (Table , entry 12). Unfortunately, the reactions resulted in lower yields at different ratios of donor and acceptor when the energy donor was replaced with K-2 (Table , entries 13-15). In addition, when the reaction was carried out in various organic solvents, chloroform afforded a high yield of 90%. As the most natural photocatalysis occurred in aqueous medium, thus we still selected water phase as the reaction solvent. Moreover, other organic solvents only gave moderate yields, or trace amounts of the desired product can be formed (Table ). Entry Photocatalyst Solvent Yield (%) [a] Reaction conditions: benzothiazole (0.2 mmol), the photocatalyst (5% mmol), diphenylphosphine oxide (1.2 mmol, 6 equiv.), solvent (2 mL), 30 W white LED, and under air at room temperature for 24 h.