Large-scale simulations of light-matter interaction in natural photosynthetic antenna complexes containing more than one hundred thousands of chlorophyll molecules, comparable with natural size, have been performed. Photosynthetic antenna complexes present in Green sulfur bacteria and Purple bacteria have been analyzed using a radiative non-Hermitian Hamiltonian, well-known in the field of quantum optics, instead of the widely used dipole−dipole Frenkel Hamiltonian. This approach allows us to study ensembles of emitters beyond the small volume limit (system size much smaller than the absorbed wavelength), where the Frenkel Hamiltonian fails. When analyzed on a large scale, such structures display superradiant states much brighter than their single components. An analysis of the robustness to static disorder and dynamical (thermal) noise shows that exciton coherence in the whole photosynthetic complex is larger than the coherence found in its parts. This provides evidence that the photosynthetic complex as a whole plays a predominant role in sustaining coherences in the system even at room temperature. Our results allow a better understanding of natural photosynthetic antennae and could drive experiments to verify how the response to electromagnetic radiation depends on the size of the photosynthetic antenna.

Valzelli, A., Boschetti, A., Mattiotti, F., Kargol, A., Green, C., Borgonovi, F., Luca Celardo, A. G., Large Scale Simulations of Photosynthetic Antenna Systems: Interplay of Cooperativity and Disorder, <<JOURNAL OF PHYSICAL CHEMISTRY. B, CONDENSED MATTER, MATERIALS, SURFACES, INTERFACES & BIOPHYSICAL>>, 2024; 2024 (128): 9643-9655. [doi:10.1021/acs.jpcb.4c02406] [https://hdl.handle.net/10807/305082]

Large Scale Simulations of Photosynthetic Antenna Systems: Interplay of Cooperativity and Disorder

Mattiotti, Francesco;Borgonovi, Fausto
Penultimo
Supervision
;
2024

Abstract

Large-scale simulations of light-matter interaction in natural photosynthetic antenna complexes containing more than one hundred thousands of chlorophyll molecules, comparable with natural size, have been performed. Photosynthetic antenna complexes present in Green sulfur bacteria and Purple bacteria have been analyzed using a radiative non-Hermitian Hamiltonian, well-known in the field of quantum optics, instead of the widely used dipole−dipole Frenkel Hamiltonian. This approach allows us to study ensembles of emitters beyond the small volume limit (system size much smaller than the absorbed wavelength), where the Frenkel Hamiltonian fails. When analyzed on a large scale, such structures display superradiant states much brighter than their single components. An analysis of the robustness to static disorder and dynamical (thermal) noise shows that exciton coherence in the whole photosynthetic complex is larger than the coherence found in its parts. This provides evidence that the photosynthetic complex as a whole plays a predominant role in sustaining coherences in the system even at room temperature. Our results allow a better understanding of natural photosynthetic antennae and could drive experiments to verify how the response to electromagnetic radiation depends on the size of the photosynthetic antenna.
2024
Inglese
Valzelli, A., Boschetti, A., Mattiotti, F., Kargol, A., Green, C., Borgonovi, F., Luca Celardo, A. G., Large Scale Simulations of Photosynthetic Antenna Systems: Interplay of Cooperativity and Disorder, <<JOURNAL OF PHYSICAL CHEMISTRY. B, CONDENSED MATTER, MATERIALS, SURFACES, INTERFACES & BIOPHYSICAL>>, 2024; 2024 (128): 9643-9655. [doi:10.1021/acs.jpcb.4c02406] [https://hdl.handle.net/10807/305082]
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/10807/305082
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