Significant Enhancement of the Upconversion Emission in Highly Er(3+) -Doped Nanoparticles at Cryogenic Temperatures.
Significant Enhancement of the Upconversion Emission in Highly Er(3+) -Doped Nanoparticles at Cryogenic Temperatures.
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高浓度 Er3 掺杂纳米粒子在低温下的上转换发射显着增强
DOI：
10.1002/anie.202217100
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发表时间：
2023-02-06
影响因子：
16.6
通讯作者：
Zhang, Hong
中科院分区：
文献类型：
--
作者：
Tu, Langping;Wu, Kefan;Luo, Yongshi;Wang, Enhui;Yuan, Jun;Zuo, Jing;Zhou, Ding;Li, Bin;Zhou, Jiajia;Jin, Dayong;Zhang, Hong
相对较低的效率是镧系元素掺杂的上转换纳米颗粒（UCNPs）应用的瓶颈。近年来实现的高水平掺杂策略并没有像预期的那样提高效率。有人认为交叉弛豫（CR）是无害的上转换。本文将联合收割机理论模拟和光谱学方法相结合，研究了CR在Er 3+高掺杂（HD）UCNPs上转换过程中的作用。发现如果有目的地抑制CR，则可以显著提高上转换效率。具体来说，我们实验表明，通过引入低温环境（40 K）抑制CR增强了两个数量级以上的上转换发射。 这项工作不仅阐明了CR的本质及其不可忽视的不利影响，而且为提高上转换效率提供了新的视角。其结果可直接应用于低温成像和大范围温度传感。通过引入低温环境来抑制有害的交叉弛豫，富含Er 3+的核-壳结构的上转换强度可以显著提高超过100倍，同时对红色到绿色发射比的调制超过50倍。
Relatively low efficiency is the bottleneck for the application of lanthanide‐doped upconversion nanoparticles (UCNPs). The high‐level doping strategy realized in recent years has not improved the efficiency as much as expected. It is argued that cross relaxation (CR) is not detrimental to upconversion. Here we combine theoretical simulation and spectroscopy to elucidate the role of CR in upconversion process of Er3+ highly doped (HD) UCNPs. It is found that if CR is purposively suppressed, upconversion efficiency can be significantly improved. Specifically, we demonstrate experimentally that inhibition of CR by introducing cryogenic environment (40 K) enhances upconversion emission by more than two orders of magnitude. This work not only elucidates the nature of CR and its non‐negligible adverse effects, but also provides a new perspective for improving upconversion efficiency. The result can be directly applied to cryogenic imaging and wide range temperature sensing. By introducing a cryogenic environment to suppress the harmful cross relaxation, the upconversion intensity of Er3+‐rich core–shell structures can be significantly improved over 100‐fold, together with an over 50‐fold modulation on the red‐to‐green emission ratio.
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