Mechanochemical Preparation and Self-Assembly of Protein:Dye Hybrids for White Luminescence

[Image: see text] Protein nanofibrils (PNFs) functionalized with multiple dyes are prepared by a combination of mechanochemistry and liquid-phase self-assembly. The three employed dyes are Fluorescent Brightener 378 (F378), 2-butyl-6-(butylamino)-1H-benzo[de]isoquinoline-1,3(2H)-dione (Fluorol 555), and Nile red (NR). F378 acts as the donor with Fluorol 555 as the acceptor. F555 in turn acts as the donor and NR as the acceptor. This enables a FRET cascade that enables conversion of UV light to white light. The efficiency of FRET can be influenced by the details of the self-assembly process. If proteins milled with different dyes are mixed prior to self-assembly, nanofibrils are formed containing all three dyes, thus favoring FRET processes. By tuning the ratio of the three luminescent dyes, PNF dispersions are obtained that display bright white light emission. Moreover, the PNF dispersions can be converted into white luminescent films and gels where the PNFs may help to organize dye molecules. Additionally, the PNF materials can be employed as coatings on commercial LEDs, enabling emission of white light.