Combinatorial Discovery of Lanthanide-Doped Nanocrystals with Spectrally Pure Upconverted Emission
Combinatorial Discovery of Lanthanide-Doped Nanocrystals with Spectrally Pure Upconverted Emission
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DOI：
10.1021/nl3017994
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发表时间：
2012-07-01
期刊：
影响因子：
10.8
通讯作者：
Milliron, Delia J.
中科院分区：
文献类型：
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作者：
Chan, Emory M.;Han, Gang;Milliron, Delia J.
掺杂镧系元素离子的纳米颗粒在近红外激发下通过称为上转换的过程表现出稳定的可见光，从而实现长时间、低背景的生物成像。然而，镧系元素离子的复杂、重叠的发射光谱可能阻碍用多个上转换探针标记的样品的定量成像。在这里，我们使用多重掺杂NaYF4纳米晶体的组合筛选，以确定一系列的双重和三重掺杂的上转换纳米粒子，表现出窄，光谱纯的发射光谱在各种可见波长。然后，我们开发了一个全面的动力学模型验证了我们广泛的实验数据集。应用这个模型，我们阐明了产生光谱纯发射的能量传递机制。这些机制表明了在镧系元素掺杂的上转换纳米颗粒中产生鲁棒的颜色调谐的电子能级结构的设计规则。由此产生的材料将是有用的背景无干扰成像和生物过程的跟踪。
Nanoparticles doped with lanthanide ions exhibit stable and visible luminescence under near-infrared excitation via a process known as upconversion, enabling long-duration, low-background biological imaging. However, the complex, overlapping emission spectra of lanthanide ions can hinder the quantitative imaging of samples labeled with multiple upconverting probes. Here, we use combinatorial screening of multiply doped NaYF4 nanocrystals to identify a series of doubly and triply doped upconverting nanoparticles that exhibit narrow, spectrally pure emission spectra at various visible wavelengths. We then developed a comprehensive kinetic model validated by our extensive experimental data set. Applying this model, we elucidated the energy transfer mechanisms giving rise to spectrally pure emission. These mechanisms suggest design rules for electronic level structures that yield robust color tuning in lanthanide-doped upconverting nanoparticles. The resulting materials will be useful for background-free multicolor imaging and tracking of biological processes.