Time-Dependent Atomistic Simulations of the CP29 Light-Harvesting Complex
arXiv:2104.05034 · doi:10.1063/5.0053259
Abstract
Light harvesting as the first step in photosynthesis is of prime importance for life on earth. For a theoretical description of photochemical processes during light harvesting, spectral densities are key quantities. They serve as input functions for modeling the excitation energy transfer dynamics and spectroscopic properties. Herein, a recently developed procedure is applied to determine the spectral densities of the pigments in the minor antenna complex CP29 of photosystem II which has recently gained attention because of its active role in non-photochemical quenching processes in higher plants. To this end, the density functional based tight binding (DFTB) method has been employed to enable simulation of the ground state dynamics in a quantum-mechanics/molecular mechanics (QM/MM) scheme for each chlorophyll pigment. Subsequently, the time-dependent extension of the long-range corrected DFTB approach has been used to obtain the excitation energy fluctuations along the ground-state trajectories also in a QM/MM setting. From these results the spectral densities have been determined and compared for different force fields and to spectral densities from other light-harvesting complexes. In addition, the excitation energy transfer in the CP29 complex has been studied using ensemble-average wave packet dynamics.
References in corpus (8)
- Long-lived quantum coherence in photosynthetic complexes at physiological temperature
- Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer
- Excitons in a Photosynthetic Light-Harvesting System: A Combined Molecular Dynamics/Quantum Chemistry and Polaron Model Study
- Atomistic study of the long-lived quantum coherences in the Fenna-Matthews-Olson complex
- On the alternatives for bath correlators and spectral densities from mixed quantum-classical simulations
- Local protein solvation drives direct down-conversion in phycobiliprotein PC645 via incoherent vibronic transport
- Chebyshev Hierarchical Equations of Motion for Systems with Arbitrary Spectral Densities and Temperatures
- Long-range coherent energy transport in Photosystem II