Hu Jialing, Zhao Fei, Ling Huan, Zhang Yunxiang, Liu Qian
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University Shanghai 200438 China
Nanoscale Adv. 2024 Apr 12;6(11):2945-2953. doi: 10.1039/d4na00198b. eCollection 2024 May 29.
Single-particle detection and sensing, powered by Förster resonance energy transfer (FRET), offers precise monitoring of molecular interactions and environmental stimuli at a nanometric resolution. Despite its potential, the widespread use of FRET has been curtailed by the rapid photobleaching of traditional fluorophores. This study presents a robust single-particle FRET platform utilizing upconversion nanoparticles (UCNPs), which stand out for their remarkable photostability, making them superior to conventional organic donors for energy transfer-based assays. Our comprehensive research demonstrates the influence of UCNPs' size, architecture, and dye selection on the efficiency of FRET. We discovered that small particles (∼14 nm) with a Yb-enriched outermost shell exhibit a significant boost in FRET efficiency, a benefit not observed in larger particles (∼25 nm). 25 nm UCNPs with an inert NaLuF shell demonstrated a comparable level of emission enhancement FRET as those with a Yb-enriched outermost shell. At the single-particle level, these FRET-enhanced UCNPs manifested an upconversion green emission intensity that was 8.3 times greater than that of their unmodified counterparts, while maintaining notable luminescence stability. Our upconversion FRET system opens up new possibilities for developing more effective high-brightness, high-sensitivity single-particle detection, and sensing modalities.
由Förster共振能量转移(FRET)驱动的单粒子检测与传感技术,能够以纳米级分辨率精确监测分子间相互作用和环境刺激。尽管具有潜力,但传统荧光团的快速光漂白限制了FRET的广泛应用。本研究提出了一种强大的单粒子FRET平台,该平台利用上转换纳米粒子(UCNP),其突出特点是具有卓越的光稳定性,使其在基于能量转移的检测中优于传统有机供体。我们的综合研究证明了UCNP的尺寸、结构和染料选择对FRET效率的影响。我们发现,最外层富含镱的小颗粒(约14纳米)的FRET效率显著提高,而较大颗粒(约25纳米)则未观察到这种优势。具有惰性NaLuF壳层的25纳米UCNP表现出与最外层富含镱的UCNP相当的发射增强FRET水平。在单粒子水平上,这些FRET增强的UCNP表现出的上转换绿色发射强度比未修饰的对应物高8.3倍,同时保持了显著的发光稳定性。我们的上转换FRET系统为开发更有效的高亮度、高灵敏度单粒子检测和传感模式开辟了新的可能性。