Zhou Xuezhe, Xia Xiaojing, Smith Bennett E, Lim Matthew B, Bard Alexander B, Pant Anupum, Pauzauskie Peter J
Fundamental & Computational Sciences Directorate , Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.
ACS Appl Mater Interfaces. 2019 Jun 26;11(25):22817-22823. doi: 10.1021/acsami.8b17271. Epub 2019 Jun 17.
The development of upconversion nanomaterials for many photonic applications requires a detailed understanding of their radiative lifetimes that in turn depend critically on local environmental conditions. In this work, hexagonal (β-phase) sodium-yttrium-fluoride (NaYF) nanowires (NWs) were synthesized and substitutionally co-doped with a luminescent solid solution of trivalent erbium and ytterbium ions. A single-beam laser trapping instrument was used in tandem with a piezo-controlled, variable-temperature stage to precisely vary the nanowire's distance from the substrate. The spontaneous photoluminescence lifetime of the S → I transition from Er ions was observed to change by >60% depending on the ions' separation distance from a planar (water/glass) dielectric interface. The S state lifetime is observed to increase by a factor of 1.62 ± 0.01 as the distance from the quartz coverslip increases from ∼0 nm to ∼40 μm. Less significant changes in the luminescence lifetime (≤10%) were observed over a temperature range between 25 and 50 °C. The distance dependence of the lifetime is interpreted quantitatively in the context of classical electromagnetic coupling between Er ions within the nanowire and the adjacent dielectric interface. We also demonstrate potential applications of the NaYF NWs for both controlling and probing temperatures at nanometer scales by integrating them within a poly(dimethylsiloxane) composite matrix.
开发用于多种光子应用的上转换纳米材料需要详细了解其辐射寿命,而辐射寿命又严重依赖于局部环境条件。在这项工作中,合成了六方(β相)氟化钠钇(NaYF)纳米线,并将三价铒离子和镱离子的发光固溶体进行了替代共掺杂。将单光束激光捕获仪器与压电控制的可变温度台串联使用,以精确改变纳米线与基底的距离。观察到,根据铒离子与平面(水/玻璃)介电界面的分离距离,从铒离子的S→I跃迁的自发光致发光寿命变化超过60%。当与石英盖玻片的距离从约0 nm增加到约40μm时,观察到S态寿命增加了1.62±0.01倍。在25至50°C的温度范围内,观察到发光寿命的变化不太显著(≤10%)。在纳米线内的铒离子与相邻介电界面之间的经典电磁耦合背景下,对寿命的距离依赖性进行了定量解释。我们还通过将NaYF纳米线整合到聚二甲基硅氧烷复合基质中,展示了其在纳米尺度上控制和探测温度的潜在应用。