Tuning emission color of molecular fluorophores is of fundamental interest as it directly reflects the manipulation of excited states at the quantum mechanical level. Despite recent progress in molecular design and engineering on single fluorophores, a systematic methodology to obtain multicolor emission in aggregated or solid states, which gives rise to practical implications, remains scarce. In this study, we present a general strategy to continuously tune the emission color of a single-fluorophore aggregate by polymerization-mediated through-space charge transfer (TSCT). Using a library of well-defined styrenic donor (D) polymers grown from an acceptor (A) fluorophore by controlled radical polymerization, we found that the solid-state emission color can be fine-tuned by varying three molecular parameters: (i) the monomer substituent, (ii) the end groups of the polymer, and (iii) the polymer chain length. Experimental and theoretical investigations reveal that the color tunability originates from the structurally dependent TSCT process that regulates charge transfer energy.
Monodisperse rice-like Ni 2+ -doped β-Ga 2 O 3 nanostructures were phase-controllably synthesized via hydrothermal route and subsequent calcination. The detailed phase, composition and morphology were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM) and high resolution transmission electron microscopy (HRTEM), which showed the rice-like β-Ga 2 O 3 nanostructures were assembled with nanorods with a diameter of ~50 nm along their entire length. The phase formation and transition behavior of β-Ga 2 O 3 nanocrystals were investigated, and a possible crystal growth mechanism of rice-like GaOOH nanostructure was proposed.Photoluminescence (PL) spectra indicated that Ni 2+ -doped β-Ga 2 O 3 phosphors exhibit a broadband near-infrared emission (1200~1600 nm). Besides, the magnetic property was also investigated, revealing the Ni 2+ -doped β-Ga 2 O 3 nanocrystals a ferromagnetic nature. The single phase Ni 2+ -doped β-Ga 2 O 3 nanocrystals endowed with optical and magnetic bifunctional properties have promising potential application in the fields of optical communication, biological diagnosis and magnetic information storage, etc.
Graphical AbstractBroadband near-infrared emission (1200~1600 nm) and ferromagnetic properties was detected from single phase Ni 2+ -doped β-Ga 2 O 3 nanocrystals via mediated phase-controlled synthesis. The realization of optical-magnetic bifunctional nanocrystals is meaningful for the application in high-accuracy communications, bio-labels, etc.
<p>Tuning emission color of molecular fluorophores is of fundamental interest as it directly reflects the manipulation of excited states at the quantum-mechanical level. Despite recent progress in molecular design and engineering on single fluorophores, a systematic methodology to obtain multicolor emission in aggregated or solid states, which gives rise to practical implications in different fields, remains scarce. This is due to the complex interplay between the charge-transfer (CT) and singlet excitons. In this study, we present a general strategy to tune the emission color of a single-fluorophore aggregate by controlled radical polymerization-mediated charge transfer. Using a library of well-defined styrenic donor (D) polymers grown from an acceptor (A) fluorophore by atom transfer radical polymerization (ATRP), we found that the solid-state emission color can be fine-tuned by varying three molecular parameters: (i) the monomer substituent, (ii) the end-groups of the polymer, and (iii) the polymer chain length. Experimental and theoretical investigations reveal that the color tunability originates from the structurally dependent through-space charge transfer (TSCT) process that regulates CT energy. We further demonstrate that the polymer systems can be processed into thin films enabling versatile photolithography.</p>
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