标题： 振动电子激子理论的单重态裂变。 II. 相关三重态对态的二维光谱检测 显示英文标题

标题： Vibronic exciton theory of singlet fission. II. Two-dimensional spectroscopic detection of the correlated triplet pair state

摘要： 单线态裂变是一种分子过程，通过该过程，光子被有效转化为低能三重态激子对，有望作为提高光伏器件效率的一种手段。 在本系列的前一篇文章中，我们提出了一个振动子理论来描述单线态裂变，这一理论受到之前实验和理论研究的启发，这些研究表明振动子耦合在裂变动力学中起着重要作用。 在此，我们扩展了模型以模拟二维电子光谱，通过与五环芳烃晶体最近测量结果的比较，进一步验证了该理论。 此外，通过这种光谱模拟，我们提供了关于相关三重态对态本质的新见解，这是裂变过程中的第一个产物中间体。 特别是，我们解决了文献中关于其向更高能级三重态的光学跃迁的识别、能量和跃迁偶极矩存在分歧的问题。 显示英文摘要

摘要： Singlet fission, the molecular process through which photons are effectively converted into pairs of lower energy triplet excitons, holds promise as a means of boosting photovoltaic device efficiencies. In the preceding article of this series, we formulated a vibronic theory of singlet fission, inspired by previous experimental and theoretical studies suggesting that vibronic coupling plays an important role in fission dynamics. Here, we extend our model in order to simulate two-dimensional electronic spectra, through which the theory is further validated based on a comparison to recent measurements on pentacene crystals. Moreover, by means of such spectral simulations, we provide new insights into the nature of the correlated triplet pair state, the first product intermediate in the fission process. In particular, we address a disagreement in the literature regarding the identification, energies, and transition dipole moments of its optical transitions towards higher-lying triplet states.