Dissipation Pathways in a Photosynthetic Complex

Gustin, Ignacio; Kim, Chang Woo; Franco, Ignacio

doi:10.1021/acs.jpclett.5c02945

Dissipation Pathways in a Photosynthetic Complex

Journal Article · Fri Dec 12 00:00:00 EST 2025 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.5c02945· OSTI ID:3010494

^[1]; Kim, Chang Woo ^[2]; ^[1]

Univ. of Rochester, NY (United States)
Chonnam National Univ., Gwangju (Korea, Republic of)

Determining how energy flows within and between molecules is crucial for understanding chemical reactions, material properties, and even vital processes such as photosynthesis. While the general principles of energy transfer are well established, elucidating the specific molecular pathways by which energy is funneled remains challenging, as it requires tracking energy flow in complex molecular environments. Here, we demonstrate how photon excitation energy is partially dissipated in the light-harvesting Fenna–Matthews–Olson (FMO) complex, mediating the excitation energy transfer from light-harvesting chlorosomes to the photosynthetic reaction center in green sulfur bacteria. Specifically, we isolate the contribution of the protein and specific vibrational modes of the pigment molecules to the energy dynamics. For this, we introduce an efficient computational implementation of a recently proposed theory of dissipation pathways for open quantum systems, based on second-order perturbation theory in the electronic couplings. Using it and a state-of-the-art FMO model with highly structured and chromophore-specific spectral densities, we demonstrate that energy dissipation is dominated by low-frequency modes (<800 cm^–1) as their energy range is near-resonance with the energy gaps between electronic states of the pigments. We identify the most important modes for dissipation to be in-plane breathing modes (∼200 cm^–1) of the bacteriochlorophylls in the complex. Conversely, far-detuned intramolecular vibrations with higher frequencies (>800 cm^–1) play no role in dissipation. Interestingly, the FMO complex first needs to borrow energy from the environment to release excess photonic energy, indicating that the energy exchange between the system and thermal environment is not strictly unidirectional in time but involves a transient thermally activated step. Beyond their fundamental value, these insights can guide the development of artificial light-harvesting devices and, more broadly, engineer environments for chemical and quantum control tasks.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Rochester, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0025334

OSTI ID:: 3010494

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 51 Vol. 16; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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