论文标题
通过振动共振陷阱介导的能量传输
Trap Mediated Energy Transport via Vibronic Resonance
论文作者
论文摘要
通过振动共振控制能量传递是一种有趣的可能性。对于完全捕获其在驱动能量转移中的作用，必须精确处理非绝热振动耦合。但是，扩展系统中振动的精确处理是昂贵的，有时需要过度简化近似值以降低振动维度，并且不提供物理见解。在这里，我们为兴奋的耦合聚集体提供了有效的正常模式，这些模式将总体高维振动性哈密顿量降低到独立的一维哈密顿量。在三聚玩具模型上应用这种方法，我们展示了电子未耦合位点之间的陷阱介导的能量传输。将未偶联的位点带入振动共振中，将“陷阱”转换为“导管”以进行人口转移，同时最大程度地减少了被困的激发。可视化沿骨料正常模式的能量转移提供了非直觉的见解，特定的振动运动可以通过促进振动混合来捕获陷阱介导的能量传输。
Controlling energy transfer through vibronic resonance is an interesting possibility. Exact treatment of non-adiabatic vibronic coupling is necessary to fully capture its role in driving energy transfer. However, exact treatment of vibrations in extended systems is expensive, sometimes requiring oversimplifying approximations to reduce vibrational dimensionality, and do not provide physical insights into which specific vibrational motions promote energy transport. Here we derive effective normal modes for excitonically coupled aggregates which reduce the overall high-dimensional vibronic Hamiltonian into independent one-dimensional Hamiltonians. Applying this approach on a trimer toy model, we demonstrate trap-mediated energy transport between electronically uncoupled sites. Bringing uncoupled sites into vibronic resonance converts the `trap' into a `conduit' for population transfer, while simultaneously minimizing trapped excitations. Visualizing energy transfer along the aggregate normal modes provides non-intuitive insights into which specific vibrational motions allow for trap-mediated energy transport by promoting vibronic mixing.
