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Growing-In of Optical Coherence in the FMO Antenna Complexes

机译:FMO天线配合物中光学相干的增长

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摘要

We report on the novel effect of the growing-in of optical coherence in the FMO antenna complexes. The rise of coherence, monitored by femtosecond two-pulse photon echo spectroscopy at 1.27 K, occurs within a characteristic time of 150-250 fs after impulsive excitation at the red edge of the absorption spectrum and is accompanied by strong and long-lasting oscillations. We show that this effect cannot be explained in the framework of present theories for the photon echo formation. To account for the observations, we take into consideration a finite system-bath interaction time and develop the theory beyond the Markov limit. We show that the coherence does not follow the impulsive excitation promptly, instead its time development is delayed. General expressions are obtained for the nonlinear polarization, which can also be applied for analysis of other time-resolved experiments (three-pulse photon echoes, transient grating, transient absorption etc.). Model calculations fully support our experimental observations.
机译:我们报告了在FMO天线配合物中的光学相干性增长的新型效应。通过飞秒双脉冲光子回波光谱仪在1.27 K处监测到的相干性上升发生在吸收光谱的红色边缘上的脉冲激发后150-250 fs的特征时间内,并伴有强烈而持久的振荡。我们表明,这种影响不能在光子回波形成的当前理论框架中得到解释。考虑到这些观察结果,我们考虑了有限的系统-浴相互作用时间,并发展了超出马尔​​可夫极限的理论。我们证明了相干性并没有立即遵循脉冲激励,相反其时间发展被延迟了。获得了非线性极化的一般表达式,也可以将其用于其他时间分辨实验的分析(三脉冲光子回波,瞬态光栅,瞬态吸收等)。模型计算完全支持我们的实验观察。

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