Thermally-Limited Exciton Delocalization in Superradiant Molecular Aggregates

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• 作者：Dylan H. Arias ; Katherine W. Stone ; Sebastiaan M. Vlaming ; Brian J. Walker ; Moungi G. Bawendi ; Robert J. Silbey ; Vladimir Bulovi膰 ; Keith A. Nelson
• 刊名：The Journal of Physical Chemistry B
• 出版年：2013
• 出版时间：April 25, 2013
• 年：2013
• 卷：117
• 期：16
• 页码：4553-4559
• 全文大小：570K
• 年卷期：v.117,no.16(April 25, 2013)
• ISSN：1520-5207

文摘

We present two-dimensional Fourier transform optical spectroscopy measurements of two types of molecular J-aggregate thin films and show that temperature-dependent dynamical effects govern exciton delocalization at all temperatures, even in the presence of significant inhomogeneity. Our results indicate that in the tested molecular aggregates, even when the static structure disorder dominates exciton dephasing dynamics, the extent of exciton delocalization may be limited by dynamical fluctuations, mainly exciton鈥損honon coupling. Thus inhomogeneous dephasing may mediate the exciton coherence time whereas dynamical fluctuations mediate the exciton coherence length.