Thermally-Limited Exciton Delocalization in Superradiant Molecular Aggregates

被引：50

作者：

Arias, Dylan H. ^{[1
,2
]}

Stone, Katherine W. ^{[2
,3
]}

Vlaming, Sebastiaan M. ^{[1
,2
]}

Walker, Brian J. ^{[1
,2
]}

Bawendi, Moungi G. ^{[1
,2
]}

Silbey, Robert J. ^{[1
,2
]}

Bulovic, Vladimir ^{[2
,3
]}

Nelson, Keith A. ^{[1
,2
]}

机构：

[1] MIT, Dept Chem, Cambridge, MA 02139 USA

[2] MIT, Ctr Exciton, Cambridge, MA 02139 USA

[3] MIT, Elect Res Lab, Cambridge, MA 02139 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY B | 2013年 / 117卷 / 16期

关键词：

LINE-SHAPES; ELECTRONIC SPECTROSCOPY; RADIATIVE LIFETIME; ENERGY-TRANSFER; FLUORESCENCE; DYES; LOCALIZATION; ABSORPTION; NANOTUBES; COHERENCE;

D O I：

10.1021/jp3086717

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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-phonon coupling. Thus inhomogeneous dephasing may mediate the exciton coherence time whereas dynamical fluctuations mediate the exciton coherence length.

引用

页码：4553 / 4559

页数：7

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