Multistep Quantum Master Equation Theory for Response Functions in Four Wave Mixing Electronic Spectroscopy of Multichromophoric Macromolecules

Bulletin of the Korean chemical society

Seogjoo jang¹ 

关键词: Four wave mixing;    Response function;    Multichromophoric macromolecule;   

DOI  :  

学科分类：化学（综合）

来源: Korean Chemical Society

【 摘 要 】

This work provides an alternative derivation of third order response functions in four wave mixing spectroscopy of multichromophoric macromolecular systems considering only single exciton states. For the case of harmonic oscillator bath linearly and diagonally coupled to exciton states, closed form expressions showing all the explicit time dependences are derived. These expressions can provide more solid physical basis for understanding 2- dimensional electronic spectroscopy signals. For more general cases of system-bath coupling, the quantum master equation (QME) approach is employed for the derivation of multistep time evolution equations for Green function-like operators. Solution of these equations is feasible at the level of 2nd order non-Markovian QME, and the new approach can account for inter-exciton coupling, dephasing, relaxation, and non-Markovian effects in a consistent manner.

【 授权许可】

Unknown