相干探测二维相干光谱中激子离域和激子-激子湮灭的特征
Signatures of Exciton Delocalization and Exciton-Exciton Annihilation in Fluorescence-Detected Two-Dimensional Coherent Spectroscopy
摘要：
我们提出了计算荧光检测相干二维（F-2DES）光谱的分子异源二聚体。我们比较了F-2DES技术如何不同于标准的相干检测二维（2DES）光谱测量激子离域。我们分析了这两种方法得到的零等待时间谱中的交叉峰是由哪些过程引起的。基于严格的含时微扰理论，我们研究了如何在这两种方法中不同程度的微扰贡献之间的抵消引起的交叉峰，并确定激子湮没和激子弛豫贡献的交叉峰在零等待时间的F-2DES。我们建议，时间选通荧光检测可以用来隔离湮灭贡献F-2DES检索信息相当于2DES光谱和研究湮灭贡献本身。
英文摘要：
We present calculations of the fluorescence-detected coherent two-dimensional (F-2DES) spectra of a molecular heterodimer. We compare how the F-2DES technique differs from the standard coherently detected two-dimensional (2DES) spectroscopy in measuring exciton delocalization. We analyze which processes contribute to cross-peaks in the zero-waiting-time spectra obtained by the two methods. Based strictly on time-dependent perturbation theory, we study how in both methods varying degree of cancellation between perturbative contributions gives rise to cross-peaks, and identify exciton annihilation and exciton relaxation contributions to the cross-peak in the zero-waiting-time F-2DES. We propose that time-gated fluorescence detection can be used to isolate the annihilation contribution to F-2DES both to retrieve information equivalent to 2DES spectroscopy and to study annihilation contribution itself.
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