The two-dimensional three-pulse photon echo signals from a dimer system are investigated in detail. A perturbative approach is used to calculate the response of the system via a numerical propagation of the density matrix in exciton state representation. Exciton vibrational coupling is modeled by Redfield relaxation theory. The main goal of this paper is to dissect the two-dimensional spectrum of the dimer to give better understanding of how the dynamics influence the spectral features. We will show how different Liouville pathways lead to the appearance/disappearance of diagonal and cross peaks. The inclusion of a Gaussian shaped electric field will be contrasted to the use of delta-pulses in the impulsive limit. The impulsive limit is found to be a satisfactory approximation at long population times, while at shorter times, in the pulse-overlap region, more realistic electric fields are called for.
|Journal||Physical Review B (Condensed Matter and Materials Physics)|
|Publication status||Published - 2006|
Bibliographical noteThe information about affiliations in this record was updated in December 2015.
The record was previously connected to the following departments: Chemical Physics (S) (011001060)
Subject classification (UKÄ)
- Atom and Molecular Physics and Optics