▎ 摘　　要

Carbon-based nanomaterials hold promise for eco-friendly alter-natives to heavy-metal-containing quantum dots (QDs) in optoelectronic applications. Here, boric acid-functionalized graphene quantum dots (B-GQDs) were prepared using bottom-up molecular fusion based on nitrated pyrenes and boric acid. Such B-GQDs with crystalline graphitic structures and hydrogen-bonding functionalities would be suitable model systems for unraveling the photoluminescence (PL) mechanism, while serving as versatile building blocks for supramolecular self-assembly. Unlike conventional GQDs with multiple emissive states, the B-GQDs exhibited excitation-wavelength-independent, vibronic-coupled excitonic emission. Interestingly, their PL spectra can be tuned without largely sacrificing the quantum yield (QY) due to two-dimensional self-assembly. In addition, such B-GQDs in a polystyrene matrix possessed an ultrahigh QY (similar to 90%) and large exciton binding energy (similar to 300 meV). Benefiting from broadband absorption, ultrahigh QY, and long-wavelength emission, efficient laminated luminescent solar concentrators (100 x 100 x 6.3 mm(3)) were fabricated, yielding a high power conversion efficiency (1.4%).