Gridization-Driven Mesoscale Self-Assembly of Conjugated Nanopolymers into Luminescence-Anisotropic Photonic Crystals

Organic semiconducting emitters integrated with butterfly-mimetic photonic crystals (PhCs) are fascinating for dramatic advantages over light outcoupling efficiency and multifunctional strain sensors, as well as the key step toward electrically pumped lasers. Herein, an unprecedentedly direct mesoscale self-assembly into 1D PhCs is reported through a covalently gridization-driven approach of wide-bandgap conjugated polymers. A simple solvent-casting procedure allows for in situ self-assembly of the state-of-the-art conjugated nanopolymer, poly{[4-(octyloxy)-9,9-diphenylfluoren-2,7-diyl]grid}-co-{[5-(octyloxy)-9,9-diphenylfluoren-2,7-diyl]grid} (PODPFG), into well-defined multilayer architectures with an excellent toughness (30–40 J m^–3). This ordered meso-architecture shows a typical Bragg–Snell diffraction behavior to testify the PhC nature, along with a high effective refractive index (1.80–1.88) and optical transmittance (85–87%). The PhC films also exhibit an angle-dependent blue/green photoluminescence switching, an electroluminescence efficiency enhancement by 150–250%, and an amplified spontaneous emission enhancement with ultralow waveguide loss coefficient (2.60 cm^–1). Gridization of organic semiconductors offers promising opportunities for cross-scale morphology-directed molecular design in multifunctional organic mechatronics and intelligences.