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Controllable Formation of Luminescent Carbon Quantum Dots Mediated by the Fano Resonances Formed in Oligomers of Gold Nanoparticles

Rapid and controllable formation of fluorescent carbon quantum dots (CQDs) is highly desirable in the fields of nanophotonics and biophotonics. Here, a novel strategy for creating CQDs, which emit white light efficiently under the excitation of either laser light or a mercury lamp, is proposed and demonstrated. The luminescent CQDs are generated by irradiating a poly(vinyl alcohol) (PVA) film doped with dense gold nanoparticles (AuNPs) with femtosecond laser pulses. The creation of CQDs from PVA is a two‐step dehydration process mediated by AuNPs which act not only as heat sources but also as catalytic agents. The formation of CC, CC, and CO bonds is confirmed by infrared Fourier transformation spectroscopy and X‐ray photoelectron spectroscopy. It is revealed both numerically and experimentally that a spatially localized temperature distribution at the deep subwavelength scale can be achieved in oligomers of AuNPs by resonantly exciting the Fano resonances formed in the oligomers of AuNPs, enabling the generation of CQDs with small diameters. As one of the potential applications, it is demonstrated that optical display and optical data storage with ultralow energy can be realized by selectively introducing luminescent CQDs in the AuNP/PVA film.