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

  title={Energy flow in the Photosystem I supercomplex: Comparison of approximative theories with DM-HEOM},
  author={Tobias Kramer and Matthias Noack and Jeffrey R. Reimers and Alexander Reinefeld and Mirta Rodr'iguez and Shiwei Yin},
  journal={Chemical Physics},
Two-Dimensional Electronic Spectroscopy of a Minimal Photosystem I Complex Reveals the Rate of Primary Charge Separation.
Redfield-Förster energy transfer computations showed that the kinetics of the elementary steps involved in the overall trapping of PSI is limited by transfer from these red-shifted pigments, which implies activationless electron transfer in PSI.
The structure of a red-shifted photosystem I reveals a red site in the core antenna
A chimeric Photosystem I complex in Synechocystis PCC 6803 that shows enhanced absorption in the red spectral region and identifies the structural elements that constitute red sites that can expand the absorption spectrum of oxygenic photosynthetic and potentially modulate light harvesting efficiency.
Effect of disorder and polarization sequences on two-dimensional spectra of light-harvesting complexes
This work shows by detailed theoretical calculations how 2DES of the Fenna–Matthews–Olson complex are affected by rotational and conformational disorder of the chromophores.
Formally exact simulations of mesoscale exciton dynamics in molecular materials†
It is demonstrated that the adaptive HOPS (adHOPS) methodology provides a formally exact and size-invariant scaling algorithm for simulating mesoscale quantum dynamics.
Electronic energy transfer in biomacromolecules
Electronic energy transfer is widely used as a molecular ruler to interrogate the structure of biomacromolecules, and performs a key task in photosynthesis by transferring collected energy through
Recent advances in single-molecule spectroscopy studies on light-harvesting processes in oxygenic photosynthesis
Photosynthetic light-harvesting complexes (LHCs) play a crucial role in concentrating the photon energy from the sun that otherwise excites a typical pigment molecule, such as chlorophyll-a, only
Computational spectroscopy of complex systems.
  • T. Jansen
  • Chemistry
    The Journal of chemical physics
  • 2021
This Perspective will review the computational spectroscopy methods that have been developed and applied for infrared and visible spectroscopies in the condensed phase and discuss some of the questions that this has allowed answering.
Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM).
The HEOM theory has been used to treat systems of practical interest, in particular, to account for various linear and nonlinear spectra in molecular and solid state materials, to evaluate charge and exciton transfer rates in biological systems, to simulate resonant tunneling and quantum ratchet processes in nanodevices, and to explore quantum entanglement states in quantum information theories.
Enhanced TEMPO Algorithm for Quantum Path Integrals with Off-Diagonal System-Bath Coupling: Applications to Photonic Quantum Networks.
Multitime system correlation functions are relevant in various areas of physics and science, dealing with system-bath interaction including spectroscopy and quantum optics, where many of these


Chlorophyll Excitations in Photosystem I of Synechococcus elongatus
The Qy excitation energies of the 96 chlorophyll molecules in photosystem I of Synechococcus elongatus, both in and out of their protein environments, were obtained by using the semiempirical INDO/S
From Structure to Dynamics: Modeling Exciton Dynamics in the Photosynthetic Antenna PS1
Frequency domain spectra of the photosystem I (PS1) of Synechococcus elongatus are measured in a wide temperature range and explained in an exciton model based on the recently determined X-ray
Excitation energy transfer rates: comparison of approximate methods to the exact solution
We have evaluated excitation energy transfer rates in photosyntetic complexes using the exact HEOM method and various approximate methods frequently used in the literature, namely, the F\"orster
Robustness and Optimality of Light Harvesting in Cyanobacterial Photosystem I
An effective Hamiltonian is constructed for the chlorophyll aggregate to describe excitation transfer dynamics and spectral properties of PSI and shows that at room temperature fluctuations of site energies have little effect on the calculated excitation lifetime and quantum yield.
Efficiency of energy funneling in the photosystem II supercomplex of higher plants† †Electronic supplementary information (ESI) available: The ESI contains the parameters for the used spectral densities and details the convergence of HEOM. See DOI: 10.1039/c5sc04296h
Energy transfer in the C2S2M2 supercomplex is sensitive to structural modulations induced e.g. by the reorganization process, and is limited by the uphill transfer from CP47 to the RC core.
Exciton delocalization and transport in photosystem I of cyanobacteria Synechococcus elongates: simulation study of coherent two-dimensional optical signals.
Electronic excitations and the optical properties of the photosynthetic complex PSI are analyzed using an effective exciton model and signatures of exciton cooperative dynamics in nonchiral and chirality-induced two-dimensional photon-echo signals are identified.
Assignment of the Qy absorption spectrum of photosystem-I from Thermosynechococcus elongatus based on CAM-B3LYP calculations at the PW91-optimized protein structure.
The Qy absorption spectrum of Photosystem-I from Thermosynecochoccus elongatus is calculated using the CAM-B3LYP density functional and INDO schemes based on a quantum-mechanically refined structure for the entire photosystem obtained using the PW91 density functional.
Modeling of excitation dynamics in photosynthetic light-harvesting complexes: exact versus perturbative approaches
We compare various theoretical approaches that are frequently used for modeling the excitation dynamics in photosynthetic light-harvesting complexes. As an example, we calculate the dynamics in the