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2015-12-08

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Si us plau utilitzeu sempre aquest identificador per citar o enllaçar aquest document: https://hdl.handle.net/2445/175614

Theoretical characterization of the spectral density of the water-soluble chlorophyll-binding protein from combined quantum mechanics/molecular mechanics molecular dynamics simulations

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Recurs relacionat

https://doi.org/10.1021/acs.jctc.5b00891

Resum

Over the past decade, both experimentalists and theorists have worked to develop methods to describe pigment-protein coupling in photosynthetic light-harvesting complexes in order to understand the molecular basis of quantum coherence effects observed in photosynthesis. Here we present an improved strategy based on the combination of quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulations and excited-state calculations to predict the spectral density of electronic-vibrational coupling. We study the water-soluble chlorophyll-binding protein (WSCP) reconstituted with Chl a or Chl b pigments as the system of interest and compare our work with data obtained by Pieper and co-workers from differential fluorescence line-narrowing spectra (Pieper et al. J. Phys. Chem. B 2011, 115 (14), 4042−4052). Our results demonstrate that the use of QM/MM MD simulations where the nuclear positions are still propagated at the classical level leads to a striking improvement of the predicted spectral densities in the middle- and high-frequency regions, where they nearly reach quantitative accuracy. This demonstrates that the so-called 'geometry mismatch' problem related to the use of low-quality structures in QM calculations, not the quantum features of pigments high-frequency motions, causes the failure of previous studies relying on similar protocols. Thus, this work paves the way toward quantitative predictions of pigment-protein coupling and the comprehension of quantum coherence effects in photosynthesis.

Matèries

Llum, Fotosíntesi, Química quàntica, Química física

Matèries (anglès)

Light, Photosynthesis, Quantum chemistry, Physical and theoretical chemistry

Citació

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Articles publicats en revistes (Farmàcia, Tecnologia Farmacèutica i Fisicoquímica)

Citació

ROSNIK, Andreana M. R and CURUTCHET BARAT, Carles E. Theoretical characterization of the spectral density of the water-soluble chlorophyll-binding protein from combined quantum mechanics/molecular mechanics molecular dynamics simulations. Journal of Chemical Theory and Computation. 2015. Vol. 11, num. 12, pags. 5826-5837. ISSN 1549-9618. [consulted: 20 of August of 2026]. Available at: https://hdl.handle.net/2445/175614

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