本文探讨了荧光检测的二维光谱（F-2DES）与标准相干检测2DES在测量分子异质二聚体中激子局部化的区别。通过时间依赖的修正理论，我们揭示了两种方法中交叉峰的形成原理，特别指出了激子湮灭和松弛过程对F-2DES零等待时间谱的影响。提出利用时间门控荧光检测分离激子湮灭贡献，旨在获取等效于2DES的信息并研究这一过程。
摘要：
Incoherently detected coherent multidimensional spectroscopy is rapidly gaining popularity, promising a different application range and sensitivity than its traditional counterpart. While measuring the same response, the two methods are not equivalent. 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 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. Strictly on the basis of time-dependent perturbation theory, we study how in both methods the varying degree of cancellation between perturbative contributions gives rise to cross-peaks and we 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 the annihilation contribution itself.
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