Full Microscopic Simulations Uncover Persistent Quantum Effects in Primary Photosynthesis
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arXiv
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| Auteurs principaux: | , , , , , |
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| Format: | Preprint |
| Publié: |
2025
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| _version_ | 1866911232597950464 |
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| author | Lorenzoni, Nicola Lacroix, Thibaut Lim, James Tamascelli, Dario Huelga, Susana F. Plenio, Martin B. |
| author_facet | Lorenzoni, Nicola Lacroix, Thibaut Lim, James Tamascelli, Dario Huelga, Susana F. Plenio, Martin B. |
| contents | The presence of quantum effects in photosynthetic excitation energy transfer has been intensely debated over the past decade. Nonlinear spectroscopy cannot unambiguously distinguish coherent electronic dynamics from underdamped vibrational motion, and rigorous numerical simulations of realistic microscopic models have been intractable. Experimental studies supported by approximate numerical treatments that severely coarse-grain the vibrational environment have claimed the absence of long-lived quantum effects. Here, we report the first non-perturbative, accurate microscopic model simulations of the Fenna-Matthews-Olson photosynthetic complex and demonstrate the presence of long-lived excitonic coherences at 77 K and room temperature, which persist on picosecond time scales, similar to those of excitation energy transfer. Furthermore, we show that full microscopic simulations of nonlinear optical spectra are essential for identifying experimental evidence of quantum effects in photosynthesis, as approximate theoretical methods can misinterpret experimental data and potentially overlook quantum phenomena. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2503_17282 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Full Microscopic Simulations Uncover Persistent Quantum Effects in Primary Photosynthesis Lorenzoni, Nicola Lacroix, Thibaut Lim, James Tamascelli, Dario Huelga, Susana F. Plenio, Martin B. Chemical Physics Quantum Physics The presence of quantum effects in photosynthetic excitation energy transfer has been intensely debated over the past decade. Nonlinear spectroscopy cannot unambiguously distinguish coherent electronic dynamics from underdamped vibrational motion, and rigorous numerical simulations of realistic microscopic models have been intractable. Experimental studies supported by approximate numerical treatments that severely coarse-grain the vibrational environment have claimed the absence of long-lived quantum effects. Here, we report the first non-perturbative, accurate microscopic model simulations of the Fenna-Matthews-Olson photosynthetic complex and demonstrate the presence of long-lived excitonic coherences at 77 K and room temperature, which persist on picosecond time scales, similar to those of excitation energy transfer. Furthermore, we show that full microscopic simulations of nonlinear optical spectra are essential for identifying experimental evidence of quantum effects in photosynthesis, as approximate theoretical methods can misinterpret experimental data and potentially overlook quantum phenomena. |
| title | Full Microscopic Simulations Uncover Persistent Quantum Effects in Primary Photosynthesis |
| topic | Chemical Physics Quantum Physics |
| url | https://arxiv.org/abs/2503.17282 |