A general strategy for tailoring upconversion luminescence in lanthanide-doped inorganic nanocrystals through local structure engineering†,Nanoscale

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A general strategy for tailoring upconversion luminescence in lanthanide-doped inorganic nanocrystals through local structure engineering†
Nanoscale ( IF 5.8 ) Pub Date : 2018-04-16 00:00:00 , DOI: 10.1039/c8nr01519h
Huhui Fu _{1,

2,

3,

4,

5} , Pengfei Peng _{1,

2,

3,

4,

5} , Renfu Li _{1,

2,

3,

4,

5} , Caiping Liu _{1,

2,

3,

4,

5} , Yongsheng Liu _{1,

2,

3,

4,

5} , Feilong Jiang _{1,

2,

3,

4,

5} , Maochun Hong _{1,

2,

3,

4,

5} , Xueyuan Chen _{1,

2,

3,

4,

5}

Affiliation

A local structure around lanthanide (Ln³⁺) emitters in Ln³⁺-doped upconversion nanocrystals (UCNCs) is of fundamental importance in tailoring their upconversion luminescence (UCL) features. However, a general strategy responsible for the local-structure-dependent UCL in Ln³⁺-doped UCNCs has not been conclusively established to date. Herein, we report a new class of alkaline zirconium fluoride-based Yb³⁺/Er³⁺ co-doped UCNCs featuring a diversity of crystallographic structures for Ln³⁺ ion doping, which thereby allow us to thoroughly understand the origin underlying the local-structure-dependent UCL of the Er³⁺ ion for the first time. We reveal that the high-symmetry crystal lattice of Yb³⁺/Er³⁺ co-doped UCNCs may incur the large UCL red-to-green intensity ratio of Er³⁺ regardless of their identical elemental compositions. In combination with the first-principles calculations, we show that such local-structure-dependent UCL of Er³⁺ is primarily due to the varied electronic band structures induced by the Yb³⁺/Er³⁺ doping in different crystallographic structures of alkaline zirconium fluorides. These findings may open up a new avenue for constructing high-quality UCNCs with a tailored UCL profile and lifetime for diverse applications.

中文翻译：

通过局部结构工程定制掺杂镧系元素的无机纳米晶体的上转换发光的一般策略†

在掺杂Ln ^3+的上转换纳米晶体（UCNCs）中，镧系元素（Ln ³⁺）发射极周围的局部结构对于调整其上转换发光（UCL）功能至关重要。但是，到目前为止，尚未确定建立负责Ln ³⁺掺杂的UCNC中依赖于局部结构的UCL的通用策略。在此，我们报告了一类新型的基于碱性氟化锆的Yb ³⁺ / Er ³⁺共掺杂UCNC，其特征在于Ln ³⁺离子掺杂的晶体结构各不相同，从而使我们能够全面了解局部分子结构的起源。 Er ^3+的结构依赖性UCL第一次。我们表明，Yb组成的高对称晶格³⁺ / ER ³⁺共掺杂UCNCs可能产生大的UCL红至绿铒强度比³⁺不论其相同的元素组合物。结合第一性原理计算，我们表明，这种依赖于局部结构的Er ^3+的UCL主要是由于Yb ³⁺ / Er ³⁺掺杂在碱性锆的不同晶体结构中诱导的电子带结构变化所致。氟化物。这些发现可能会为构建高质量的UCNC开辟新途径，这些UCNC具有量身定制的UCL配置文件和适用于各种应用的生命周期。

更新日期：2018-04-16

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