Optical Projection and Spatial Separation of Spin-Entangled Triplet Pairs from the S1 (21 Ag-) State of Pi-Conjugated Systems
Optical Projection and Spatial Separation of Spin-Entangled Triplet Pairs from the S1 (21 Ag-) State of Pi-Conjugated Systems
复制标题
Pi 共轭系统 S1 (21 Ag-) 态自旋纠缠三重态对的光学投影和空间分离
DOI：
10.1016/j.chempr.2020.09.011
复制
发表时间：
2020
期刊：
影响因子：
23.5
通讯作者：
Pandya R
中科院分区：
文献类型：
--
作者：
Pandya R
S1（21 Ag-）态是天然和合成π共轭材料的光学暗态，在光电过程中发挥作用，如能量收集，光保护和单重态裂变。然而，S1波函数的实验特征仍然很少。在这里，研究一个原型的聚合物，聚丁二炔，和类胡萝卜素，我们实验证实，S1（21 Ag-）是一个叠加态与自旋纠缠对的三重态激子（1（TT））的强贡献。然后，我们表明，使用三重态吸收跃迁的S1波函数的光学操纵允许选择性的投影的1（TT）组件到一个流形的空间分离的三重态对的寿命提高了一个数量级。我们的研究结果提供了一个统一的图片21银-状态π共轭材料，并提供了一个迄今尚未探索的途径，以创建近自由的三重态。更一般地说，我们的研究结果开辟了新的路线，利用21银动力学在单线态裂变，光生物学和分子量子技术。
The S1(21Ag–) state is an optically dark state of natural and synthetic pi-conjugated materials that plays a role in optoelectronic processes, such as energy harvesting, photoprotection, and singlet fission. Experimental characterizations of the S1wavefunction, however, have remained scarce. Here, studying an archetypal polymer, polydiacetylene, and carotenoids, we experimentally confirm that S1(21Ag–) is a superposition state with strong contributions from spin-entangled pairs of triplet excitons (1(TT)). We then show that optical manipulation of the S1wavefunction using triplet absorption transitions allows selective projection of the1(TT) component into a manifold of spatially separated triplet pairs with lifetimes enhanced by up to one order of magnitude. Our results provide a unified picture of 21Ag–states in pi-conjugated materials and provide a hitherto unexplored pathway to create near-free triplets. More generally, our findings open new routes to exploit 21Ag–dynamics in singlet fission, photobiology, and molecular quantum technologies.