Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport.

Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport.
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制定用于明确检测激子能量传输中量子相干性的光谱协议。

DOI:
10.1039/c9fd00068b
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发表时间:
2019
影响因子:
3.4
通讯作者:
A. Datta
A. Datta
中科院分区:
化学2区
文献类型:
--
作者:
M. Marcus;G. Knee;A. Datta

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量子效应在激子能量输运(EET)中的作用已经得到了密切的关注,并且实验技术越来越复杂。这种增加的复杂性需要调用相应的精细模型来拟合光谱数据,然后才能提取分子参数。然后可以研究EET中可能的量子效应,但结论在很大程度上取决于拟合的有效性和模型的准确性。为了规避这一挑战,我们提出了一个证人的量子相干EET,可以直接从双脉冲泵浦探测光谱实验数据中提取。我们提供模拟来判断我们的方法的可行性。有点违反直觉的是,我们的协议并不直接探测量子相干性,而只是通过隐式删除来间接探测。它允许没有量子相干性的经典模型被决定性地排除。
The role of quantum effects in excitonic energy transport (EET) has been scrutinised intensely and with increasingly sophisticated experimental techniques. This increased complexity requires invoking correspondingly elaborate models to fit spectroscopic data before molecular parameters can be extracted. Possible quantum effects in EET can then be studied, but the conclusions are strongly contingent on the efficacy of the fitting and the accuracy of the model. To circumvent this challenge, we propose a witness for quantum coherence in EET that can be extracted directly from two-pulse pump-probe spectroscopy experimental data. We provide simulations to judge the feasibility of our approach. Somewhat counterintuitively, our protocol does not probe quantum coherence directly, but only indirectly through its implicit deletion. It allows for classical models with no quantum coherence to be decisively ruled out.
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