Extracting accurate information from triplet–triplet annihilation upconversion data with a mass-conserving kinetic model
Extracting accurate information from triplet–triplet annihilation upconversion data with a mass-conserving kinetic model
复制标题
使用质量守恒动力学模型从三重态-三重态湮灭上转换数据中提取准确的信息
DOI：
10.1039/d2cp03986a
复制
发表时间：
2022
影响因子：
3.3
通讯作者：
Fourkas, John T.
中科院分区：
文献类型：
--
作者：
Kalpattu, Abhishek;Dilbeck, Tristan;Hanson, Kenneth;Fourkas, John T.
三重态-三重态湮没上转换(TTA-UC)是一种在能量采集和光能产生技术等领域显示出良好应用前景的过程。TTA-UC系统的辐照度相关性能通常使用图形分析来测量，而不是使用详细的模型。此外，TTA-UC的动力学模型很少包含质量守恒，这是一种在实验相关条件下可能产生重要后果的现象。我们给出了一个解析的、质量守恒的TTA-UC动力学模型，并证明了质量守恒约束一般不能被忽略。该模型考虑了TTA-UC数据的饱和。饱和度使阈值辐照度ith的解释变得复杂，这是一种流行的性能指标。我们提出了两个可供选择的整体表现优劣系数。最后，我们表明，我们的模型可以稳健地拟合来自各种敏化TTA-UC系统的实验数据，从而能够直接和准确地确定ith和我们提出的性能度量。我们采用这种拟合程序，使用文献中的数据对这些指标进行基准测试和比较。
Triplet–triplet annihilation upconversion (TTA-UC) is a process that shows promise for applications such as energy-harvesting and light-generation technologies. The irradiance dependent performance of TTA-UC systems is typically gauged using a graphical analysis, rather than a detailed model. Additionally, kinetic models for TTA-UC rarely incorporate mass conservation, which is a phenomenon that can have important consequences under experimentally relevant conditions. We present an analytical, mass-conserving kinetic model for TTA-UC, and demonstrate that the mass-conservation constraint cannot generally be ignored. This model accounts for saturation in TTA-UC data. Saturation complicates the interpretation of the threshold irradiance Ith, a popular performance metric. We propose two alternative figures of merit for overall performance. Finally, we show that our model can robustly fit experimental data from a wide variety of sensitized TTA-UC systems, enabling the direct and accurate determination of Ith and of our proposed performance metrics. We employ this fitting procedure to benchmark and compare these metrics, using data from the literature.