Abstract
We present simulations of 3rd and 5th order multidimensional time-dependent signals of a molecular trimer. The developed model allows for the simulation of both signal types within one theoretical framework. We therefore extended standard Redfield theory of exciton migration by a new term to include the process of exciton-exciton annihilation.
Highlights
We present simulations of 3rd and 5th order multidimensional time-dependent signals of a molecular trimer
Dynamics involving multiple excitons can be studied by another 3rd order signal, called 2Q-2D electronic spectroscopy, and measured along kIII= k1+k2-k3
Both 3rd and 5th order signals are modeled in a resonantly coupled molecular complex consisting of three subunits, each possessing two energy levels and an associated transition dipole moment μi
Summary
Dynamics involving multiple excitons can be studied by another 3rd order signal, called 2Q-2D electronic spectroscopy, and measured along kIII= k1+k2-k3. We present simulations of 3rd and 5th order multidimensional time-dependent signals of a molecular trimer. The developed model allows for the simulation of both signal types within one theoretical framework.
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