Climent Clàudia, Casanova David, Feist Johannes, Garcia-Vidal Francisco J
Departamento de Física Teórica de la Materia Condensada and Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, 28049 Madrid, Spain.
Donostia International Physics Centre (DIPC), 20018 Donostia, Euskadi, Spain.
Cell Rep Phys Sci. 2022 Apr 20;3(4):100841. doi: 10.1016/j.xcrp.2022.100841.
Polaritons are unique hybrid light-matter states that offer an alternative way to manipulate chemical processes. In this work, we show that singlet fission dynamics can be accelerated under strong light-matter coupling. For superexchange-mediated singlet fission, state mixing speeds up the dynamics in cavities when the lower polariton is close in energy to the multiexcitonic state. This effect is more pronounced in non-conventional singlet fission materials in which the energy gap between the bright singlet exciton and the multiexcitonic state is large ( eV). In this case, the dynamics is dominated by the polaritonic modes and not by the bare-molecule-like dark states, and, additionally, the resonant enhancement due to strong coupling is robust even for energetically broad molecular states. The present results provide a new strategy to expand the range of suitable materials for efficient singlet fission by making use of strong light-matter coupling.
极化激元是独特的光与物质的混合态，为操纵化学过程提供了一种替代方法。在这项工作中，我们表明在强光与物质耦合下，单线态裂变动力学可以加速。对于超交换介导的单线态裂变，当下极化激元的能量与多激子态相近时，态混合会加速腔中的动力学过程。这种效应在非常规单线态裂变材料中更为明显，其中明亮单线态激子与多激子态之间的能隙较大（ 电子伏特）。在这种情况下，动力学由极化激元模式主导，而非类似裸分子的暗态主导，此外，即使对于能量较宽的分子态，强耦合引起的共振增强也很显著。目前的结果提供了一种新策略，即通过利用强光与物质耦合来扩大适用于高效单线态裂变的材料范围。
