Theory of Photosynthetic Energy and Charge Transfer
Theory of Photosynthetic Energy and Charge Transfer
Matching Funds - Oberösterreich
Disciplines
Biology (20%); Chemistry (40%); Physics, Astronomy (40%)
Keywords
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Energy Transfer,
Electron Transfer,
Photosynthesis,
Density Matrix Theory,
Electrostatics,
Optical Spectra
In photosynthesis carbon dioxid, water and sun light are used to synthesize sugar, which is an important building block of plants. Nature has developed a complicated machinery in order to catalyze this light- driven reaction. Many microscopic details are not fully understood yet. In this project we aim at deciphering the structure-function relationships of the primary energy and charge transfer reactions of photosynthesis. Sun light absorbed in light-harvesting antennae is transferred to the photosynthetic reaction center, where it is used to drive electron transfer reactions. In photosystem II water is split into oxygen, electrons and protons. The oxygen is released, the electrons are shuttled to photosystem I, where they are stored in the chemical bonds of NADPH. The protons drive a molecular motor, the ATPase, which generates ATP, the energy of which is used later in the carbohydrate synthesis. The collection of light energy occurs with a quantum efficiency close to 100 %, that is from 100 absorbed photons on average more than 95 reach the photosynthetic reaction center and drive a chain of primary electron transfer reactions. The latter initiate the chemical reactions for the storage of the solar energy. The origin of the high quantum efficiency of the primary excitation energy and charge transfer reactions is given by the pigment-protein coupling. The optically active pigments (chlorophylls and carotenoids) are held in an optimal distance and orientation for energy- and charge transfer by the protein scaffold. Moreover, the protein also controls the electronic energies of the pigments by electrostatic interactions. In this way, a directed energy transfer towards the reaction center becomes possible. In the present project we want to decipher the underlying molecular details on the basis of the atomic structure of various photosynthetic pigment-protein complexes. In our previous project we have developed a multi- scale approach and investigated the energy transfer in small subunits of the photosynthetic apparatus. Here, we will study the interplay of energy and charge transfer in larger parts of the photosystems. For this purpose, on one hand, it will be necessary to incorporate charge transfer states in our description and on the other hand we need to develop efficient calculation schemes for the description of optical experiments on large systems containing a few hundred pigments. On this basis, we want to understand the molecular building principles of photosynthetic complexes, that will be helpful also in the construction of artificial solar energy converting systems like organic solar cells.
- Universität Linz - 100%
- Nicholas Cox, Australian National University - Australia
- Jessica M. Anna, University of Pennsylvania - USA
- Jasper J. Van Thor, Imperial College London - United Kingdom
Research Output
- 107 Citations
- 13 Publications
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2023
Title Short-Range Effects in the Special Pair of Photosystem II Reaction Centers: The Nonconservative Nature of Circular Dichroism DOI 10.1021/acs.jpclett.3c02693 Type Journal Article Author Gemeinhardt F Journal The Journal of Physical Chemistry Letters Pages 11758-11767 Link Publication -
2023
Title Time-resolved circular dichroism of excitonic systems: theory and experiment on an exemplary squaraine polymer DOI 10.1039/d3sc01674a Type Journal Article Author Ress L Journal Chemical Science Pages 9328-9349 Link Publication -
2023
Title Living on the edge: light-harvesting efficiency and photoprotection in the core of green sulfur bacteria DOI 10.1039/d3cp01321a Type Journal Article Author Klinger A Journal Physical Chemistry Chemical Physics Pages 18698-18710 Link Publication -
2021
Title Semiclassical Modified Redfield and Generalized Förster Theories of Exciton Relaxation/Transfer in Light-Harvesting Complexes: The Quest for the Principle of Detailed Balance DOI 10.1021/acs.jpcb.1c01479 Type Journal Article Author Renger T Journal The Journal of Physical Chemistry B Pages 6406-6416 Link Publication -
2021
Title Reply to: Is the debate over grana stacking formation finally solved? DOI 10.1038/s41477-021-00881-6 Type Journal Article Author Müh F Journal Nature Plants Pages 279-281 -
2022
Title Towards a quantitative description of excitonic couplings in photosynthetic pigment–protein complexes: quantum chemistry driven multiscale approaches DOI 10.1039/d1cp03566e Type Journal Article Author Friedl C Journal Physical Chemistry Chemical Physics Pages 5014-5038 Link Publication -
2022
Title Exact simulation of pigment-protein complexes unveils vibronic renormalization of electronic parameters in ultrafast spectroscopy DOI 10.1038/s41467-022-30565-4 Type Journal Article Author Caycedo-Soler F Journal Nature Communications Pages 2912 Link Publication -
2022
Title Signatures of intramolecular vibrational and vibronic Qx–Qy coupling effects in absorption and CD spectra of chlorophyll dimers DOI 10.1007/s11120-022-00946-3 Type Journal Article Author Seibt J Journal Photosynthesis Research Pages 19-37 Link Publication -
2022
Title Role of Environmental Dynamic Polarizability in Static Excited State Properties of Embedded Molecular Systems: Application to Disordered Fluorographene Systems DOI 10.1021/acs.jpcc.2c06779 Type Journal Article Author Sla´Ma V Journal The Journal of Physical Chemistry C Pages 381-392 -
2024
Title Theory of 2D electronic spectroscopy of water soluble chlorophyll-binding protein (WSCP): Signatures of Chl b derivate DOI 10.1063/5.0200876 Type Journal Article Author Riedl M Journal The Journal of Chemical Physics Pages 184114 -
2020
Title Normal mode analysis of spectral density of FMO trimers: Intra- and intermonomer energy transfer DOI 10.1063/5.0027994 Type Journal Article Author Klinger A Journal The Journal of Chemical Physics Pages 215103 Link Publication -
2020
Title Static Disorder in Excitation Energies of the Fenna–Matthews–Olson Protein: Structure-Based Theory Meets Experiment DOI 10.1021/acs.jpclett.0c03123 Type Journal Article Author Chaillet M Journal The Journal of Physical Chemistry Letters Pages 10306-10314 Link Publication -
2024
Title Towards understanding the crystallization of photosystem II: influence of poly(ethylene glycol) of various molecular sizes on the micelle formation of alkyl maltosides DOI 10.1007/s11120-024-01079-5 Type Journal Article Author Müh F Journal Photosynthesis Research Pages 1-17 Link Publication