人工分子光收集器中长寿命相干性的振动起源
Vibronic origin of long-lived coherence in an artificial molecular light harvester
摘要：
自然和人工光收集过程最近获得了新的兴趣。生物系统的光谱信号中的持久相干性的签名已经被反复观察到，尽管它们的起源是一个正在进行的辩论的问题，因为目前还不清楚如何避免由于与这种系统中的噪声环境的相互作用而导致的相干性损失。在这里，我们报告的实验和理论验证的相干激子振动（电子振动）耦合的起源持久的相干性在人工光收获机，分子J-聚集。在这个宏观对齐的管状系统中，偏振控制2D光谱提供了一个不拥挤和特定的光学响应，作为深入理论描述的理想基础。我们推导出的解析表达式表明，在一般条件下，电子振动耦合导致延长激发态相干。
英文摘要：
Natural and artificial light harvesting processes have recently gained new interest. Signatures of long lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of ongoing debate, as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton-vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.
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