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Plasmonic Dual-Enhancement and Precise Color Tuning of Gold Nanorod@SiO2 Coupled Core-Shell-Shell Upconversion Nanocrystals

机译:金纳米棒@ SiO2偶联核-壳-壳上转换纳米晶体的等离子双增强和精确的色彩调节。

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The last decade has witnessed the remarkable research progress of lanthanide-doped upconversion nanocrystals (UCNCs) at the forefront of promising applications. However, the future development and application of UCNCs are constrained greatly by their underlying shortcomings such as significant nonradiative processes, low quantum efficiency, and single emission colors. Here a hybrid plasmonic upconversion nanostructure consisting of a GNR@SiO2 coupled with NaGdF4:Yb3+, Nd3+@ NaGdF4: Yb3+, Er3+@NaGdF4 core-shell-shell UCNCs is rationally designed and fabricated, which exhibits strongly enhanced UC fluorescence (up to 20 folds) and flexibly tunable UC colors. The experimental findings show that controlling the SiO2 spacer thickness enables readily manipulating the intensity ratio of the Er3+ red, green, and blue emissions, thereby allowing us to achieve the emission color tuning from pale yellow to green upon excitation at 808 nm. Electrodynamic simulations reveal that the tunable UC colors are due to the interplay of plasmon-mediated simultaneous excitation and emission enhancements in the Er3+ green emission yet only excitation enhancement in the blue and red emissions. The results not only provide an upfront experimental design for constructing hybrid plasmonic UC nanostructures with high efficiency and color tunability, but also deepen the understanding of the interaction mechanism between the Er3+ emissions and plasmon resonances in such complex hybrid nanostructure.
机译:在过去的十年中,镧系元素掺杂的上转换纳米晶体(UCNC)的研究取得了令人瞩目的研究,其应用前景十分广阔。但是,UCNCs的潜在缺陷极大地限制了UCNCs的未来开发和应用,这些缺陷包括显着的非辐射过程,低量子效率和单一发射色。在这里,由GNR @ SiO2结合NaGdF4:Yb3 +,Nd3 + @ NaGdF4:Yb3 +,Er3 + @ NaGdF4核-壳-壳UCNC组成的混合等离子体激元上转换纳米结构是经过合理设计和制造的,具有较强的UC荧光(可达20倍) )和灵活可调的UC颜色。实验结果表明,控制SiO2间隔层的厚度可以轻松控制Er3 +红色,绿色和蓝色发射的强度比,从而使我们能够在808 nm激发时实现从浅黄色到绿色的发射颜色调谐。电动力学仿真表明,可调谐UC颜色是由于等离子激元介导的Er3 +绿色发射中的同时激发和发射增强相互作用,而仅是蓝色和红色发射中的激发增强相互作用。结果不仅为构建高效,颜色可调的杂化等离子体UC纳米结构提供了前期实验设计,而且加深了对这种复杂杂化纳米结构中Er3 +发射与等离子体共振的相互作用机理的理解。

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