Alleviating NIR-II emission quenching in ring-fused fluorophore via manipulating dimer populations for superior fluorescence imaging

Résumé fourni par la source

Emission quenching resulting from fluorophore aggregation has long been a significant challenge in optimizing emission-based technologies, such as fluorescence imaging and optoelectronic devices. Alleviating this quenching in aggregates is crucial, yet progress is impeded by the limited understanding of the nature and impact of aggregates on emission. Here, we elucidate the critical role of dimeric aggregate (dimer) in alleviating second near-infrared (NIR-II, 900-1700 nm) emission quenching from ring-fused fluorophore 4F for superior fluorescence imaging. Spectral decomposition and molecular dynamics simulations demonstrate the predominance of dimer populations in 4F aggregates. Notably, dimers exhibit significantly weaker emission but intense intermolecular nonradiative (interNR) decay compared to monomers, as demonstrated by ultrafast spectra and quantum calculation. Therefore, the predominant population of dimers with weak emission and pronounced interNR feature underlies the emission quenching in 4F aggregates. This discovery guides the preparation of ultrabright NIR-II 4F nanofluorophore (4F NP3s) by decreasing dimer populations, which show 5-fold greater NIR-II brightness than indocyanine green, enabling superior resolution in visualizing blood vessels. This work offers valuable insights into aggregation-caused quenching, with broad implications extending far beyond NIR-II fluorescence imaging.

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