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基于外延生长技术构建不同结构特性的核壳结构已成为调控稀土掺杂微纳晶体材料发光特性的有效技术手段之一。为此，本文基于多次外延生长并引入NaYF4中间隔离层，构建了具有壳层独立发光特性NaYF4: 50%Yb3+/2%Tm3+@ NaYF4@NaYF4: 20%Yb3+/2%Er3+@NaYF4@NaYbF4: 2%Er3+多层微米核壳晶体。在980 nm激光激发下，借助共聚焦显微光谱测试系统，通过改变单颗粒微米晶体的激发位置，研究了单颗粒核壳微米晶体不同微区内的发光和能量传递特性。实验结果表明：在相邻发光层之间引入NaYF4惰性壳，不仅可实现单颗粒微米晶体区域内发光的调控，且可有效抑制了各壳层离子间的相互作用，实现了各壳层的多彩独立发射。同时，基于单颗粒核壳微米晶体不同区域内多彩发射特性，构建具有信息可调的微纳光子学条形码。由此可见，本文所构建具有区域化可调发射的微米核壳结构，可在不同的激发条件下实现其发光的多彩可调，其丰富光谱指纹信息为单颗粒微米材料在光学防伪领域中的应用提供了新的途径。The construction of core-shell structures with different structural properties based on the epitaxial growth technique has become an effective technique for regulating the luminescence properties of micro/nanocrystals. In order to obtain richer spectral information, this work attempts to prepare NaYF4:50%Yb3+/2%Tm3+@NaYF4@ NaYF4:20%Yb3+/2%Er3+@NaYF4@NaYbF4:2%Er3+multilayered core-shell microcry- stals by using multiple epitaxial growth with the introduction of surface modifiers and controlling their reaction conditions. From the XRD and SEM results, it is evident that the core-shell microcrystals possess a pure hexagonal crystal structure in the form of a disk.The microdisk has a thickness of about 2.32 μm with a diameter of about 28.31μm. The upconversion luminescence characteristics of different single microcrystal structures were investigated by a confocal microspectroscopy system. In order to achieve the selective excitation and emission of a single microcrystal, the spatial distribution of luminescent ions can be controlled through the introduction of an intermediate isolation layer. Under 980 nm laser excitation, different excitation sites of the single microdisk exhibit different upconversion emission characteristics. The significant blue (450 nm and 475 nm), red (648 nm) and green (524 nm and 540 nm) emissions are observed, mainly originating from Tm3+ ions and Er3+ radiative transitions. Meanwhile, the red and blue upconversion emission intensities of the microcrystals were improved by using various shell layers. In addition, the luminescence and energy-transfer features of single microcrystals were explored by varying the excitation position. The experimental results demonstrate that the incorporation of NaYF4 inert shells between luminescent layers can regulate luminescence and prevent ion interactions. By utilizing the spectral fingerprint data of dopant ions in various shell layers, we created customizable micro-nano photonic barcodes and employed them for optical anti-counterfeiting detection. This study explores the use of constructed core-shell structures with luminescent tunable micron core-shell structures to achieve diverse spectral information and maintain stability through their structural properties. Thus, this core-shell structure offers a novel approach for utilizing upconversion luminescent microcrystals in micro- and nanophotonics for anti-counterfeiting and display purposes.
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Keywords:
- upconversion luminescence /
- core-shell microcrystals /
- single particles /
- luminescence regulation /
- photonics barcodes
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