Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 133, Issue 1, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3442415
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Funding
- Grant Agency of the Czech Republic [202/07/P245]
- Ministry of Education of the Czech Republic [MSM 0021620835]
- National Science Foundation [CHE-0745892]
- National Institutes of Health [GM59230]
- Direct For Mathematical & Physical Scien [0745892] Funding Source: National Science Foundation
- Division Of Chemistry [0745892] Funding Source: National Science Foundation
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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. (C) 2010 American Institute of Physics. [doi:10.1063/1.3442415]
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