Restricting molecular motion of fluorophores is the most direct and effective approach to creating highly emissive fluorescent materials.However,attempts to limit molecular motion of conventional fluorophores in aqueo...Restricting molecular motion of fluorophores is the most direct and effective approach to creating highly emissive fluorescent materials.However,attempts to limit molecular motion of conventional fluorophores in aqueous environments often encounter undesired aggregation-caused quenching(ACQ).To address this challenge,this study presents an innovative design of a water-soluble supramolecular scaffold with a rigidmicrodomain,achieved by assembling a cyclic peptide-diblock copolymer conjugate into cylindrical nanoparticles,where the rigid microdomain is provided by the hydrophobic polymer segment with a high glass transition temperature.Supramolecular fluorophores(termed as Supra-fluorophores)are constructed by noncovalently dispersing fluorophores within the rigid microenvironment of the scaffold through a simple coassembly approach,effectively mitigating molecular motion and ACQ.This strategy accommodates a wide range of fluorophores,resulting in Supra-fluorophores with fluorescence quantum yields up to 71.6%and volume-normalized brightness reaching 19,910 M−1 cm−1 nm−3.Furthermore,increased rigidity significantly reduces dynamic exchange among assemblies by three orders of magnitude,thereby generating kinetically trapped Supra-fluorophores that exhibit minimal dye crosstalk upon mixing.This approach demonstrates substantial potential for advanced bioimaging applications,such as multicolor cell labeling,real-time tracking,and high-resolution cellular imaging.展开更多
基金the assistance of SUSTech Core Research Facilities,and CSNS for the allocation of beam time(grant nos.P0121122200005 and P0124052700001).
文摘Restricting molecular motion of fluorophores is the most direct and effective approach to creating highly emissive fluorescent materials.However,attempts to limit molecular motion of conventional fluorophores in aqueous environments often encounter undesired aggregation-caused quenching(ACQ).To address this challenge,this study presents an innovative design of a water-soluble supramolecular scaffold with a rigidmicrodomain,achieved by assembling a cyclic peptide-diblock copolymer conjugate into cylindrical nanoparticles,where the rigid microdomain is provided by the hydrophobic polymer segment with a high glass transition temperature.Supramolecular fluorophores(termed as Supra-fluorophores)are constructed by noncovalently dispersing fluorophores within the rigid microenvironment of the scaffold through a simple coassembly approach,effectively mitigating molecular motion and ACQ.This strategy accommodates a wide range of fluorophores,resulting in Supra-fluorophores with fluorescence quantum yields up to 71.6%and volume-normalized brightness reaching 19,910 M−1 cm−1 nm−3.Furthermore,increased rigidity significantly reduces dynamic exchange among assemblies by three orders of magnitude,thereby generating kinetically trapped Supra-fluorophores that exhibit minimal dye crosstalk upon mixing.This approach demonstrates substantial potential for advanced bioimaging applications,such as multicolor cell labeling,real-time tracking,and high-resolution cellular imaging.
