Luminescence and Transport Behavior in Incommensurately Modulated CaGd2(MoO4)4:Yb/Er

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry Letters Pub Date : 2024-11-06 DOI:10.1021/acs.jpclett.4c0255410.1021/acs.jpclett.4c02554
Yinghan Wang, Zeyue Zhang, Guohong Cai, Jingxie Xiong, Zhengren Tao, Chunhai Wang, Junliang Sun* and Shi Ye*, 
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Abstract

The phenomenon of thermal quenching of luminescence can significantly compromise the efficiency of luminescent materials, a process accompanied by the generation of substantial phonon populations. While plenty of models for elucidating this behavior have been proposed, the crucial role of phonon transport has largely been neglected, particularly in the enigmatic incommensurate scheelite structure with good luminescence performance. In this study, we delve into the thermal quenching dynamics of the near-infrared emission in the incommensurately modulated CaGd2(MoO4)4:Yb/Er system. Our comprehensive investigation reveals distinct evolutionary patterns in electrical conductivity, luminescence intensity, thermal conductivity, and Raman scattering at varying temperature regimes. Notably, we have determined that thermally induced ion migration, occurring above ∼300 °C, serves as a pivotal trigger for the activation of all phonons and the enhancement of phonon–defect scattering within this incommensurate framework. This phenomenon not only diminishes the thermal conductivity but also accelerates the multiphonon relaxation of the Er3+ emission levels, culminating in a marked thermal quenching of luminescence. This work illuminates the thermal quenching mechanism of luminescence by focusing on phonon scattering dynamics, providing critical insights for the design of thermally robust near-infrared luminescent materials, which are essential for the advancement of optical amplification systems.

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不可比调制的 CaGd2(MoO4)4:Yb/Er 中的发光和传输行为
发光的热淬灭现象会严重影响发光材料的效率,这一过程伴随着大量声子群的产生。虽然已经提出了大量模型来阐明这种行为,但声子输运的关键作用在很大程度上被忽视了,尤其是在具有良好发光性能的神秘不互变白钨矿结构中。在本研究中,我们深入研究了非共相调制 CaGd2(MoO4)4:Yb/Er 体系中近红外发射的热淬灭动力学。我们的全面研究揭示了不同温度条件下电导率、发光强度、热导率和拉曼散射的不同演化模式。值得注意的是,我们已经确定,发生在 ∼300 °C以上的热诱导离子迁移是激活所有声子的关键触发因素,并增强了这种不相称框架内的声子-缺陷散射。这种现象不仅降低了热导率,还加速了 Er3+ 发射水平的多声子弛豫,最终导致发光的明显热淬灭。这项研究通过重点研究声子散射动力学,阐明了发光的热淬灭机制,为设计热稳定性近红外发光材料提供了重要的启示,这对光学放大系统的发展至关重要。
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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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