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

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Summary

Introduction

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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