Luminescence Decay Dynamics and Trace Biomaterials Detection Potential of Surface-Functionalized Nanoparticles.
Luminescence Decay Dynamics and Trace Biomaterials Detection Potential of Surface-Functionalized Nanoparticles.
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DOI：
10.1021/jp8065647
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发表时间：
2008-10-22
期刊：
影响因子：
--
通讯作者：
Chen W
中科院分区：
文献类型：
--
作者：
Cheng KH;Aijmo J;Ma L;Yao M;Zhang X;Como J;Hope-Weeks LJ;Huang J;Chen W
我们研究了两种表面功能化的纳米粒子，聚（乙二醇）双（羧甲基）醚包覆的LaF 3：Ce，Tb（~20 nm）和巯基乙酸包覆的ZnS/Mn（~5 nm）的发光衰减和痕量生物材料检测潜力。在UV激发下，这些纳米颗粒在溶液中分别在540和597 nm处发射荧光峰。荧光成像显示，这些纳米颗粒针对沉积在各种无孔固体基底上的指纹中的微量生物材料。高度有序的，微观汗孔内的指纹的摩擦脊被标记具有良好的空间分辨率的纳米粒子在铝和聚甲基戊烯基板上，但不是在玻璃或石英。在溶液中，这些纳米颗粒表现出多组分荧光衰减，分辨寿命范围从纳米到微秒，涂层LaF 3：Ce，Tb和ZnS：Mn的平均寿命分别为~24和130 µs。长微秒衰减成分与在或接近纳米颗粒的核表面的发射体相关，所述核表面对纳米颗粒的尺寸、表面官能化和溶剂暴露敏感。当纳米颗粒结合到固体基质的表面上并处于干燥状态时，观察到微秒衰减寿命的减少，这表明结合和溶剂去除后表面涂层环境的变化。在干燥状态下，表面结合的ZnS：Mn在石英、铝和聚甲基戊烯上的平均衰减寿命分别为约60、30和11 µs。这些值仍然比大多数底物的典型荧光衰减背景长2个数量级（例如，对于聚甲基戊烯，约为0.36 µs）。我们得出结论，涂层ZnS：锰纳米粒子作为一种无毒标记剂，在纳米法医应用中用于超灵敏、时间门控、痕量证据检测，具有很大的前景。
We have studied the luminescence decay and trace biomaterials detection potential of two surface-functionalized nanoparticles, poly(ethylene glycol) bis(carboxymethyl) ether-coated LaF3:Ce,Tb (~20 nm) and thioglycolic acid-coated ZnS/Mn (~5 nm). Upon UV excitation, these nanoparticles emitted fluorescence peaking at 540 and 597 nm, respectively, in solution. Fluorescence imaging revealed that these nanoparticles targeted the trace biomaterials from fingerprints that were deposited on various nonporous solid substrates. Highly ordered, microscopic sweat pores within the friction ridges of the fingerprints were labeled with good spatial resolutions by the nanoparticles on aluminum and polymethylpentene substrates, but not on glass or quartz. In solution, these nanoparticles exhibited multicomponent fluorescence decays of resolved lifetimes ranging from nano-to microseconds and of average lifetimes of ~24 and 130 µs for the coated LaF3:Ce,Tb and ZnS:Mn, respectively. The long microsecond-decay components are associated with the emitters at or near the nanocrystal core surface that are sensitive to the size, surface-functionalization, and solvent exposure of the nanoparticles. When the nanoparticles were bound to the surface of a solid substrate and in the dried state, a decrease in the microsecond decay lifetimes was observed, indicative of a change in the coating environment of the nanocrystal surface upon binding and solvent removal. The average decay lifetimes for the surface-bound ZnS:Mn in the dried state were ~60, 30, and 11 µs on quartz, aluminum, and polymethylpentene, respectively. These values were still 2 orders of magnitude longer than the typical fluorescence decay background of most substrates (e.g., ~0.36 µs for polymethylpentene) in trace forensic evidence detections. We conclude that coated ZnS: Mn nanoparticles hold great promise as a nontoxic labeling agent for ultrasensitive, time-gated, trace evidence detections in nanoforensic applications.
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