标题： 用纯态自适应层次表征Peierls振动在单重态裂变中的作用 显示英文标题

标题： Characterizing the Role of Peierls Vibrations in Singlet Fission with the Adaptive Hierarchy of Pure States

摘要： 单线态裂变是一种现象，其中单线态激子转化为两个三线态激子，对扰动电子态之间耦合的振动（即佩尔斯振动）敏感。 在比二聚体更大的单线态裂变模型中，精确模拟的不便缩放限制了对佩尔斯振动的处理仅限于近似方法。 在本信中，我们将形式上精确的、降低缩放比例的纯态自适应层次结构（adHOPS）方法推广，以考虑霍尔斯坦和佩尔斯振动，并研究N,N'-双(2-苯乙基)-3,4,9,10-芘二甲酰亚胺（EP-PDI）中的单线态裂变。 我们发现，佩尔斯振动通过生成支持建设性干涉的关联电荷转移介导路径来加速单线态裂变。 最后，我们将这种单线态裂变模型扩展到EP-PDI的线性链，以证明佩尔斯振动可以在100纳米尺度上加速单线态介导的三线态传输。 显示英文摘要

摘要： Singlet fission, a phenomenon in which a singlet exciton is converted to two triplet excitons, is sensitive to vibrations that perturb couplings between electronic states (i.e., Peierls vibrations). In singlet fission models larger than dimers, the inconvenient scaling of exact simulations has limited treatment of Peierls vibrations to approximate methods. In this letter, we generalize the formally exact, reduced-scaling adaptive Hierarchy of Pure States (adHOPS) method to account for both Holstein and Peierls vibrations and study singlet fission in N,N'-Bis(2-phenylethyl)-3,4,9,10-perylenedi-carboximide (EP-PDI). We find that Peierls vibrations accelerate singlet fission by generating correlated charge transfer-mediated pathways that support constructive interference. Finally, we extend this singlet fission model to a linear chain of EP-PDI to demonstrate that Peierls vibrations can accelerate singlet-mediated triplet transport on the 100-nm scale.