Ray Krishanu, Badugu Ramachandram, Lakowicz Joseph R
Center for Fluorescence Spectroscopy, University of Maryland School of Medicine, Department of Biochemistry and Molecular Biology, 725 West Lombard Street, Baltimore, MD 21201, USA.
J Phys Chem C Nanomater Interfaces. 2007;111(19):7091-7097. doi: 10.1021/jp067635q.
Metal-Enhanced Fluorescence (MEF) has become an important method in biomedical sensing. In this paper, we present the distance-dependent MEF of sulforhodamine B (SRB) monolayer on silver island films (SIFs). SRB is electrostatically incorporated into the Langmuir-Blodgett (LB) layers of octadecylamine (ODA) deposited on glass and SIFs substrates. The distances between SRB and SIFs or glass surfaces are controlled by depositing a varied number of inert stearic acid (SA) spacer layers. SRB is incorporated into positively charged LB layers of ODA by immersing the ODA deposited substrates into aqueous solution of SRB. Dye incorporated ODA layers with 10 nm separation distance from the SIFs surface show maximum metal-enhanced fluorescence intensity; ~7-fold increase in intensity as compared to that from the glass surface. The corresponding enhancement factor is reduced with increasing or decreasing the probe distance from the SIFs surface. Additionally, SRB on SIF surfaces show reduced lifetimes. We observed the shortest lifetime from the SRB with 5 nm distance from the SIF surfaces and the lifetime increased consistently with increasing the distances between the fluorophore and the SIFs surface. These observed spectral changes, increase in fluorescence intensity and decreased fluorescence lifetimes, are in accordance with the expected effects due to near-field interactions between the silver nanoparticles and fluorophores. We have also analyzed the complex fluorescence heterogeneous decays on metallic nanostructured surfaces using continuous distributions of decay times. The decay-time distributions appear to be sensitive to the distance between the metal and fluorophore and represent the underlying heterogeneity of the samples. The present systematic study provides significant information on the effect of fluorophore distance on the metal-enhanced fluorescence phenomenon.
金属增强荧光(MEF)已成为生物医学传感中的一种重要方法。在本文中,我们展示了磺基罗丹明B(SRB)单层在银岛膜(SIFs)上的距离依赖性MEF。SRB通过静电作用被纳入沉积在玻璃和SIFs基板上的十八烷基胺(ODA)的朗缪尔-布洛杰特(LB)层中。SRB与SIFs或玻璃表面之间的距离通过沉积不同数量的惰性硬脂酸(SA)间隔层来控制。通过将沉积有ODA的基板浸入SRB水溶液中,SRB被纳入ODA带正电荷的LB层中。与SIFs表面距离为10 nm的掺入染料的ODA层显示出最大的金属增强荧光强度;与从玻璃表面测得的强度相比,强度增加了约7倍。随着探针与SIFs表面距离的增加或减少,相应的增强因子会降低。此外,SIFs表面上的SRB显示出寿命缩短。我们观察到与SIFs表面距离为5 nm的SRB的寿命最短,并且随着荧光团与SIFs表面之间距离的增加,寿命持续增加。这些观察到的光谱变化,即荧光强度增加和荧光寿命缩短,与银纳米颗粒和荧光团之间近场相互作用的预期效应一致。我们还使用衰减时间的连续分布分析了金属纳米结构表面上复杂的荧光非均匀衰减。衰减时间分布似乎对金属与荧光团之间的距离敏感,并代表了样品潜在的非均匀性。目前的系统研究提供了有关荧光团距离对金属增强荧光现象影响的重要信息。