Jones Callum M S, Biner Daniel, Misopoulos Stavros, Krämer Karl W, Marques-Hueso Jose
Institute of Sensors, Signals and Systems, Heriot-Watt University, Edinburgh, EH14 4AS, UK.
Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, 3012, Bern, Switzerland.
Sci Rep. 2021 Jul 6;11(1):13910. doi: 10.1038/s41598-021-93400-8.
Optimizing upconversion (UC) composites is challenging as numerous effects influence their unique emission mechanism. Low scattering mediums increase the number of dopants excited, however, high scattering mediums increase the UC efficiency due to its non-linear power dependency. Scattering also leads to greater thermal effects and emission saturation at lower excitation power density (PD). In this work, a photoluminescence quantum yield (PLQY) increase of 270% was observed when hexagonal NaYF:(18%)Yb,(2%)Er phosphor is in air compared to a refractive index-matched medium. Furthermore, the primary inner-filter effect causes a 94% PLQY decrease when the excitation focal point is moved from the front of the phosphor to 8.4 mm deep. Increasing this effect limits the maximum excitation PD, reduces thermal effects, and leads to emission saturation at higher excitation PDs. Additionally, self-absorption decreases the PLQY as the phosphor's thickness increases from 1 to 9 mm. Finally, in comparison to a cuboid cuvette, a 27% PLQY increase occurs when characterizing the phosphor in a cylindrical cuvette due to a lensing effect of the curved glass, as supported by simulations. Overall, addressing the effects presented in this work is necessary to both maximize UC composite performance as well as report their PLQY more reliably.
优化上转换(UC)复合材料具有挑战性,因为众多因素会影响其独特的发射机制。低散射介质会增加被激发的掺杂剂数量,然而,高散射介质因其非线性功率依赖性会提高UC效率。散射还会导致在较低激发功率密度(PD)下产生更大的热效应和发射饱和。在这项工作中,与折射率匹配介质相比,当六方相NaYF:(18%)Yb,(2%)Er荧光粉处于空气中时,观察到光致发光量子产率(PLQY)提高了270%。此外,当激发焦点从荧光粉前端移至8.4毫米深处时,主要的内滤效应会导致PLQY降低94%。增强这种效应会限制最大激发PD,降低热效应,并在较高激发PD下导致发射饱和。此外,随着荧光粉厚度从1毫米增加到9毫米,自吸收会降低PLQY。最后,模拟结果表明,与长方体比色皿相比,在圆柱形比色皿中表征荧光粉时,由于弯曲玻璃的透镜效应,PLQY会提高27%。总体而言,解决这项工作中所呈现的这些效应对于最大化UC复合材料性能以及更可靠地报告其PLQY都是必要的。