Tao Guohua
School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen 518055, China and Shenzhen Key Laboratory of New Energy Materials by Design, Peking University, Shenzhen 518055, China.
J Chem Phys. 2020 Feb 21;152(7):074305. doi: 10.1063/1.5139538.
Quantum coherence plays an important role in exciton dynamics such as singlet fission, which may be determined by molecular physical properties, including energy levels, electronic couplings, and electron-phonon couplings, and by geometric properties, including packing configuration and exciton delocalization. However, the global picture of quantum coherence in high-dimensional multistate systems is still blurred. Here, we perform nonadiabatic molecular dynamics simulation for singlet fission in tetracene clusters and demonstrate that the topology of quantum coherence in terms of the global structure of the coupled multistate system may significantly modulate fission dynamics. In particular, quantum coherence in the spin-specified models could be protected by its topological structure from external perturbations. Our work suggests that the topology of quantum coherence is indispensable in the understanding and control of quantum dynamics, which may find potential implementations to singlet fission and quantum computation.
量子相干在诸如单线态裂变等激子动力学中起着重要作用，激子动力学可能由分子物理性质决定，包括能级、电子耦合和电子 - 声子耦合，也由几何性质决定，包括堆积构型和激子离域。然而，高维多态系统中量子相干的整体情况仍然模糊不清。在此，我们对并四苯簇中的单线态裂变进行非绝热分子动力学模拟，并证明就耦合多态系统的全局结构而言，量子相干的拓扑结构可能会显著调节裂变动力学。特别地，自旋指定模型中的量子相干可以通过其拓扑结构免受外部扰动。我们的工作表明，量子相干的拓扑结构在理解和控制量子动力学方面是不可或缺的，这可能为单线态裂变和量子计算找到潜在的应用。
