Exciton coherence length fluctuations in chromophore aggregates probed by multidimensional optical spectroscopy.

Content Provider	Europe PMC
Author	Šanda, František Perlík, Václav Mukamel, Shaul
Copyright Year	2010
Abstract	The coherent third order optical response of molecular aggregates with fluctuating frequencies, couplings, and transition dipole moments is studied. We derived stochastic nonlinear exciton equations (SNEEs) by combining the quasiparticle picture of excitons with the path integral over stochastic bath paths described by the stochastic Liouville equations. Coherent two-dimensional (2D) spectra are calculated for a tetramer model system whose transition dipole orientations undergo two-state stochastic jumps on an arbitrary timescale. Correspondence between domains of ordered dipoles, which determine the exciton coherence length and the absorption peaks, is established. Signatures of domain coherence length fluctuations are observed in the cross peak dynamics of the 2D spectra in specific pulse polarization configurations.
Related Links	https://europepmc.org/backend/ptpmcrender.fcgi?accid=PMC2909306&blobtype=pdf
ISSN	00219606
Volume Number	133
DOI	10.1063/1.3442415
PubMed Central reference number	PMC2909306
Issue Number	1
PubMed reference number	20614954
Journal	The Journal of Chemical Physics [J Chem Phys]
e-ISSN	10897690
Language	English
Publisher	American Institute of Physics
Publisher Date	2010-07-01
Access Restriction	Open
Rights License	Copyright © 2010 American Institute of Physics
Content Type	Text
Resource Type	Article
Subject	Physics and Astronomy Medicine Physical and Theoretical Chemistry