Department of Materials Science and Engineering, ‡Department of Electrical and Systems Engineering, §Department of Chemistry, ∥Department of Physics and Astronomy, and ⊥Department of Bioengineering, University of Pennsylvania , Philadelphia, Pennsylvania 19104, United States.
ACS Nano. 2014 Sep 23;8(9):9482-91. doi: 10.1021/nn503675a. Epub 2014 Sep 5.
We demonstrate plasmonic enhancement of upconversion luminescence in individual nanocrystal heterodimers formed by template-assisted self-assembly. Lithographically defined, shape-selective templates were used to deterministically coassemble single Au nanorods in proximity to single hexagonal (β-phase) NaYF4:Yb(3+),Er(3+) upconversion nanophosphors. By tailoring the dimensions of the rods to spectrally tune their longitudinal surface plasmon resonance to match the 977 nm excitation wavelength of the phosphors and by spatially localizing the phosphors in the intense near-fields surrounding the rod tips, several-fold luminescence enhancements were achieved. The enhancement effects exhibited a strong dependence on the excitation light's polarization relative to the rod axis. In addition, greater enhancement was observed at lower excitation power densities due to the nonlinear behavior of the upconversion process. The template-based coassembly scheme utilized here for plasmonic coupling offers a versatile platform for improving our understanding of optical interactions among individual chemically prepared nanocrystal components.
我们展示了通过模板辅助自组装形成的单个纳米晶杂化二聚体中上转换发光的等离子体增强。通过使用光刻定义的、形状选择性的模板,我们可以在单个金纳米棒附近确定性地共组装单个六方(β 相)NaYF4:Yb(3+),Er(3+)上转换纳米荧光体。通过调整棒的尺寸,使它们的纵向表面等离激元共振光谱与荧光体的 977nm 激发波长匹配,并将荧光体在棒尖端的强近场中空间定位,实现了数倍的发光增强。增强效果强烈依赖于相对于棒轴的激发光的偏振。此外,由于上转换过程的非线性行为,在较低的激发功率密度下观察到更大的增强。这里用于等离子体耦合的基于模板的共聚方案为提高我们对单个化学制备的纳米晶组件之间的光学相互作用的理解提供了一个通用平台。