Time-Domain Line-Shape Analysis from 2D Spectroscopy to Precisely Determine Hamiltonian Parameters for a Photosynthetic Complex
Time-Domain Line-Shape Analysis from 2D Spectroscopy to Precisely Determine Hamiltonian Parameters for a Photosynthetic Complex
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利用二维光谱进行时域线形分析，精确确定光合复合体的哈密顿参数
DOI：
10.1021/acs.jpcb.0c08012
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发表时间：
2021
期刊：
影响因子：
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通讯作者：
Gardiner, Alastair T.
中科院分区：
文献类型：
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作者：
Rolczynski, Brian S.;Yeh, Shu-Hao;Navotnaya, Polina;Lloyd, Lawson T.;Ginzburg, Alan R.;Zheng, Haibin;Allodi, Marco A.;Otto, John P.;Ashraf, Khuram;Gardiner, Alastair T.
光信号来自量子态之间的相干性，其谱线宽度由相干性的退相动力学确定。使用二维电子光谱仪，我们观察到弱相干和rephasing时域信号持续到1 ps的Fenna-Matthews-Olson复杂在77 K。这些是在复合物与光相互作用一次或三次后制备的基态和激发态之间的相干性，而不是在两次相互作用后更频繁研究的零量子相干性。在这里，我们使用这些小的，但持久的信号成分，以隔离光谱贡献与窄峰，并揭示系统的本征能量。
Optical signals come from coherences between quantum states, with spectral line widths determined by the coherences’ dephasing dynamics. Using a 2D electronic spectrometer, we observe weak coherence- and rephasing-time-domain signals persisting to 1 ps in the Fenna–Matthews–Olson complex at 77 K. These are coherences between the ground and excited states prepared after the complex interacts once or three times with light, rather than zero-quantum coherences that are more frequently investigated following two interactions. Here, we use these small but persistent signal components to isolate spectral contributions with narrowed peaks and reveal the system’s eigenenergies.