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上转换发光的衰减时间。

On the decay time of upconversion luminescence.

机构信息

Department of Applied Physics, KTH Royal Institute of Technology, S-10691, Stockholm, Sweden.

出版信息

Nanoscale. 2019 Mar 14;11(11):4959-4969. doi: 10.1039/c8nr10332a.

Abstract

In this study, we systematically investigate the decay characteristics of upconversion luminescence (UCL) under anti-Stokes excitation through numerical simulations based on rate-equation models. We find that a UCL decay profile generally involves contributions from the sensitizer's excited-state lifetime, energy transfer and cross-relaxation processes. It should thus be regarded as the overall temporal response of the whole upconversion system to the excitation function rather than the intrinsic lifetime of the luminescence emitting state. Only under certain conditions, such as when the effective lifetime of the sensitizer's excited state is significantly shorter than that of the UCL emitting state and of the absence of cross-relaxation processes involving the emitting energy level, the UCL decay time approaches the intrinsic lifetime of the emitting state. Subsequently, Stokes excitation is generally preferred in order to accurately quantify the intrinsic lifetime of the emitting state. However, possible cross-relaxation between doped ions at high doping levels can complicate the decay characteristics of the luminescence and even make the Stokes-excitation approach fail. A strong cross-relaxation process can also account for the power dependence of the decay characteristics of UCL.

摘要

在本研究中,我们通过基于速率方程模型的数值模拟,系统地研究了反斯托克斯激发下上转换发光(UCL)的衰减特性。我们发现,UCL 衰减曲线通常涉及敏化剂激发态寿命、能量转移和交叉弛豫过程的贡献。因此,它应被视为整个上转换系统对激发函数的整体时间响应,而不是发光发射态的固有寿命。只有在某些条件下,例如敏化剂激发态的有效寿命明显短于 UCL 发射态的固有寿命,并且不存在涉及发射能级的交叉弛豫过程时,UCL 衰减时间才会接近发射态的固有寿命。随后,通常优选斯托克斯激发以准确量化发射态的固有寿命。然而,在高掺杂水平下掺杂离子之间可能存在的交叉弛豫会使发光的衰减特性复杂化,甚至使斯托克斯激发方法失效。强交叉弛豫过程也可以解释 UCL 衰减特性的功率依赖性。

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