Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 132, Issue 2, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3293039
Keywords
excited states; Liouville equation; master equation; perturbation theory; solvation; spectral line breadth; stochastic processes; two-dimensional spectra
Funding
- NNSF of China [20733006, 20873157, 20903101]
- Chinese Academy of Sciences [KJCX2.YW.H17]
- RGC Hong Kong [604508, 604709]
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We extend our previous study of absorption line shapes of molecular aggregates using the Liouville space hierarchical equations of motion (HEOM) method [L. P. Chen, R. H. Zheng, Q. Shi, and Y. J. Yan, J. Chem. Phys. 131, 094502 (2009)] to calculate third order optical response functions and two-dimensional electronic spectra of model dimers. As in our previous work, we have focused on the applicability of several approximate methods related to the HEOM method. We show that while the second order perturbative quantum master equations are generally inaccurate in describing the peak shapes and solvation dynamics, they can give reasonable peak amplitude evolution even in the intermediate coupling regime. The stochastic Liouville equation results in good peak shapes, but does not properly describe the excited state dynamics due to the lack of detailed balance. A modified version of the high temperature approximation to the HEOM gives the best agreement with the exact result.
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