Energy flow in the Photosystem I supercomplex: comparison of approximative theories with DM-HEOM

Abstract

We analyze the exciton dynamics in PhotosystemI from Thermosynechococcus elongatus using the distributed memory implementation of the hierarchical equation of motion (DM-HEOM) for the 96 Chlorophylls in the monomeric unit. The exciton-system parameters are taken from a first principles calculation. A comparison of the exact results with Foerster rates and Markovian approximations allows one to validate the exciton transfer times within the complex and to identify deviations from approximative theories. We show the optical absorption, linear, and circular dichroism spectra obtained with DM-HEOM and compare them to experimental results.

arXiv comment18 pages, 10 figures, fix spelling in names

References in corpus (3)

• High-performance solution of hierarchical equations of motions for studying energy-transfer in light-harvesting complexes
• Efficient calculation of open quantum system dynamics and time-resolved spectroscopy with Distributed Memory HEOM (DM-HEOM)
• Excitation energy transfer rates: comparison of approximate methods to the exact solution

Cited by in corpus (7)

• Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
• Using Fluorescence Detected Two-Dimensional Spectroscopy to Investigate Initial Exciton Delocalization Between Coupled Chromophores
• Enhanced TEMPO algorithm for quantum path integrals with off-diagonal system-bath coupling: applications to photonic quantum networks
• Simulating optical linear absorption for mesoscale molecular aggregates: an adaptive hierarchy of pure states approach
• Thermodynamic quantum Fokker-Planck equations and their application to thermostatic Stirling engine
• Effect of disorder and polarization sequences on two-dimensional spectra of light harvesting complexes
• A hierarchical equations of motion (HEOM) analog for systems with delay: illustrated on inter-cavity photon propagation