Recent progress in experimental techniques such as two-dimensional electronic spectroscopy and broadband pump-probe spectroscopy, that are capable of probing the ultrafast dynamics of excited-state wavepackets, have highlighted the existence of long-lived vibronic coherence in light-harvesting complexes. However, detailed interpretation of experimental spectra can be troublesome due to highly convoluted signals from competing energetic pathways. The ability to independently control each degree of freedom (DOF) makes theoretical analysis of these spectroscopic features a necessity.<br/>In this work, we implement the recently-developed Partial Linearized Density Matrix (PLDM) path integral method for computing nonlinear spectroscopy signals to investigate the spectral features that are characteristic of vibrationally-assisted exciton transfer in photosynthetic light harvesting complexes. The PLDM propagation method involves treating subsystem DOFs semi-classically (within the Meyer-Miller mapping formalism) while bath DOFs are treated within a truncated Wigner approximation. This method provides accurate density matrix dynamics for non-Markovian open quantum systems, from which nonlinear optical response functions can be extracted.<br/>

Signatures of vibrationally assisted exciton dynamics in two dimensional electronic spectroscopy simulations

256th National Meeting (2018)

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