Department of Physics and Astronomy, Washington State University, Pullman, Washington 99164-2814, USA.
J Chem Phys. 2012 Aug 7;137(5):054705. doi: 10.1063/1.4739295.
Here we present a model of self healing in which correlations between chromophores, as mediated by the polymer, are key to the recovery process. Our model determines the size distribution of the correlation volume using a grand canonical ensemble through a free energy advantage parameter. Choosing a healing rate that is proportional to the number of undamaged molecules in a correlated region, and a decay rate proportional to the intensity normalized to the correlation volume, the ensemble average is shown to correctly predict decay and recovery of the population of disperse orange 11-DO11 (1-amino-2-methylanthraquinone) molecules doped in PMMA polymer as a function of time and concentration as measured with amplified spontaneous emission and linear absorption spectroscopy using only three parameters that apply to the full set of data. Our model also predicts the temperature dependence of the process. One set of parameters should be characteristic of a particular polymer and dopant chromophore combination. Thus, the use of the model in determining these parameters for various materials systems should provide the data needed to test fundamental models of the underlying mechanism responsible for self healing.
在这里，我们提出了一种自修复模型，其中通过聚合物介导的发色团之间的相关性是恢复过程的关键。我们的模型通过自由能优势参数，使用巨正则系综来确定相关体积的大小分布。选择与相关区域中未损坏分子数量成正比的修复速率，以及与相关体积归一化的强度成正比的衰减速率，集合平均值被证明可以正确预测聚甲基丙烯酸甲酯（PMMA）聚合物中掺杂的分散橙 11-DO11（1-氨基-2-甲基蒽醌）分子的种群的衰减和恢复作为时间和浓度的函数，使用放大自发发射和线性吸收光谱测量，仅使用适用于完整数据集的三个参数。我们的模型还预测了该过程的温度依赖性。一组参数应该是特定聚合物和掺杂发色团组合的特征。因此，该模型在为各种材料系统确定这些参数中的使用应该提供测试负责自修复的基础机制的基本模型所需的数据。
