Related Experiment Video
Updated: Jun 11, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Exciton coherence length fluctuations in chromophore aggregates probed by multidimensional optical spectroscopy
Frantisek Sanda1, Václav Perlík, Shaul Mukamel
1Faculty of Mathematics and Physics, Institute of Physics, Charles University, Ke Karlovu 5, Prague 121 16, Czech Republic. sanda@karlov.mff.cuni.cz
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.
More Related Videos
Related Concept Videos
UV–Vis Spectroscopy: Molecular Electronic Transitions
IR Spectroscopy: Hooke's Law Approximation of Molecular Vibration
According to Hooke's law, the vibrational frequency is directly proportional to the...
Atomic Spectroscopy: Absorption, Emission, and Fluorescence
Molecular Spectroscopy: Absorption and Emission
UV–Vis Spectroscopy of Conjugated Systems
One of the factors influencing λmax is the extent of conjugation in the...
IR Absorption Frequency: Delocalization
In IR spectroscopy,...

