Theory-Guided Defect Tuning through Topochemical Reactions for Accelerated Discovery of UVC Persistent Phosphors
Theory-Guided Defect Tuning through Topochemical Reactions for Accelerated Discovery of UVC Persistent Phosphors
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理论——通过拓扑化学反应引导缺陷调节，加速 UVC 持久荧光粉的发现
DOI：
10.1002/adom.201901727
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发表时间：
2019-12-19
影响因子：
9
通讯作者：
Sun, Hong-Tao
中科院分区：
文献类型：
--
作者：
Li, Hong;Liu, Qi;Sun, Hong-Tao
长余辉发光材料因其广泛的应用而受到人们的关注。然而，迄今为止，LPP的发现很大程度上是试错的结果。在这里，理论指导的缺陷调整，通过拓扑化学反应证明了新兴的LPPs加速发现。采用第一性原理计算来确定不同缺陷态的热力学电荷跃迁能级，这有助于检查候选结构是否是合适的余辉宿主。通过拓扑化学反应合理调节缺陷的种类和浓度，发现Pr 3+掺杂LaPO4具有紫外C余辉，余辉时间超过2 h。这种策略，结合先进的表征，包括高分辨率同步辐射X射线衍射，正电子湮没寿命谱，和电子自旋共振，提出了一个自由基参与余辉机制。重要的是，它表明，这个概念可以扩展到发现更多的LPP。有人建议，理论指导的缺陷工程，使拓扑化学反应可以作为一个强大的工具，以加快发现新的LPPs更清晰的余辉机制，甚至对其他光电材料的设计的影响。
Long persistent phosphors (LPPs) have attracted enduring attention owing to their wide applications. However, the discovery of LPPs is thus far largely the results of trial and error. Here, theory-guided defect tuning through topochemical reactions is demonstrated for accelerated discovery of emerging LPPs. First-principles calculations are employed to identify the thermodynamic charge-transition levels of different defect states, which help examine whether the candidate structure is a suitable host for afterglow. Rationally tuning the species and concentrations of defects through topochemical reactions is then illustrated, which leads to discovery of Pr3+-doped LaPO4 featuring ultraviolet C afterglow with a lasting time of over 2 h. Such a strategy, in conjunction with advanced characterizations including high-resolution synchrotron X-ray diffraction, positron annihilation lifetime spectroscopy, and electron spin resonance, suggests a radical-involved afterglow mechanism. Importantly, it is illustrated that this concept can be extended for the discovery of more LPPs. It is suggested that theory-guided defect engineering enabled by topochemical reactions can be used as a powerful tool to accelerate discovery of novel LPPs with much clearer afterglow mechanisms, with implications even for the design of other optoelectronic materials.