Discrimination of Diverse Coherences Allows Identification of Electronic Transitions of a Molecular Nanoring
Discrimination of Diverse Coherences Allows Identification of Electronic Transitions of a Molecular Nanoring
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DOI：
10.1021/acs.jpclett.7b00612
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发表时间：
2017-05-18
影响因子：
5.7
通讯作者：
Zigmantas, Donatas
中科院分区：
文献类型：
--
作者：
Butkus, Vytautas;Alster, Jan;Zigmantas, Donatas
量子相干在分子系统如光合复合物的光化学功能中的作用是一个广泛争论的话题。电子和振动相干性的共存和混合被认为是观测到的长寿命相干性和高能量转移效率的原因。然而，明确的实验证据表明，不同来源的相干性在同一时间运作一直难以捉摸。在这项工作中，从六卟啉纳米环系统获得的多维光谱进行了详细的分析与理论建模的支持。我们发现了一个很大的多样性，可分离的电子，振动，和混合cohesives，并显示他们的合作，在塑造光谱响应。结果允许直接分配的电子和振动态和表征的激发动力学。具有扩展g-共轭的分子中相干性的清晰解纠缠为探索相干现象和理解它们对复杂系统功能的重要性开辟了新的途径。
The role of quantum coherence in photochemical functions of molecular systems such as photosynthetic complexes is a broadly debated topic. Coexistence and intermixing of electronic and vibrational coherences has been proposed to be responsible for the observed long-lived coherences and high energy transfer efficiency. However, clear 0 experimental evidence of coherences with different origins operating at the same time has been elusive. In this work, multidimensional spectra obtained from a six-porphyrin nanoring system are analyzed in detail with support from theoretical modeling. We uncover a great diversity of separable electronic, vibrational, and mixed coherences and show their cooperation in shaping the spectroscopic response. The results permit direct assignment of electronic and vibronic states and characterization of the excitation dynamics. The clear disentanglement of coherences in molecules with extended g-conjugation opens up new avenues for exploring coherent phenomena and understanding their importance for the function of complex systems.