固态光反应动力学和平衡中的集体行为
Collective behavior in the kinetics and equilibrium of solid-state photoreaction
摘要：
目前的兴趣在于开发在照射下变形并因此可用于光机械致动的光敏材料。这是有吸引力的，因为它可以在一定距离处受到影响，不同的频率可以用于驱动不同的模式和进行感测，并且无腐蚀的轻质光纤电缆可以在长距离上提供显著的功率。开发新的光机械材料的策略是首先在溶液中开发光活性分子，然后通过结晶或将其插入聚合物中将其以固态结合。这封信表明，动力学和光诱导的相变的性质是深刻的不同，在单分子（溶液）和固体状态下使用晶格自旋模型。在溶液中，分子独立作用，光反应遵循一级动力学。然而，在光活性分子彼此相互作用并因此在反应期间集体表现的固态中，光反应遵循成核和生长的S形动力学，如在一级相变中。此外，我们发现，光致应变的确切性质有一个关键的影响动力学，平衡，和微结构的形成。这些预测与实验观察定性一致，并为开发新的光活性材料提供了见解。
英文摘要：
There is current interest in developing photoactive materials that deform on illumination and can thus be used for photomechanical actuation. This is attractive since it can be affected at a distance, different frequencies can be used to actuate different modes and to sense, and corrosion-free lightweight fiber optic cables can deliver significant power over long distances. The strategy for developing new photomechanical materials is to first develop photoactive molecules in solution, and then to incorporate these in the solid-state either by crystallization or by inserting them into polymers. This letter shows that the kinetics and the nature of the photo-induced phase transitions are profoundly different in single molecules (solution) and in the solid state using a lattice spin model. In solution, where the molecules act independently, the photoreaction follows first-order kinetics. However, in the solid state where the photoactive molecules interact with each other and therefore behave collectively during reaction, photoreactions follow the sigmoidal kinetics of nucleation and growth as in a first-order phase transition. Further, we find that the exact nature of the photo-induced strain has a critical effect on the kinetics, equilibrium, and microstructure formation. These predictions agree qualitatively with experimental observations, and provide insights for the development of new photoactive materials.
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