ACS Publications. Most Trusted. Most Cited. Most Read

OR SEARCH CITATIONS

My Activity
Publications
CONTENT TYPES

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2018, 9, 9, 2404-2410
RETURN TO ISSUEPREVLetterNEXT

The Dynamic Origin of Color Tuning in Proteins Revealed by a Carotenoid Pigment

Cite this: J. Phys. Chem. Lett. 2018, 9, 9, 2404–2410
Publication Date (Web):April 23, 2018
https://doi.org/10.1021/acs.jpclett.8b00763
Copyright © 2018 American Chemical Society
Request reuse permissions

    Article Views

    887

    Altmetric

    -

    Citations

    24
    LEARN ABOUT THESE METRICS
    Read OnlinePDF (2 MB)
    Get e-Alerts
    Supporting Info (1)»
    SUBJECTS:

    Abstract

    Abstract Image

    Understanding the microscopic origin of the color tuning in pigment–protein complexes is a challenging yet fundamental issue in photoactive biological systems. Here, we propose a possible interpretation by using a state-of-the-art multiscale strategy based on the integration of quantum chemistry and polarizable atomistic embeddings into a dynamic description. By means of such a strategy we are able to resolve the long-standing dispute over the coloration mechanism in the crustacyanin protein. It is shown that the combination of the dynamical flexibility of the carotenoid pigments (astaxanthin) with the responsive protein environment is essential to obtain quantitative predictions of the spectral tuning. The strong linear correlation between the excitation energies and the bond length alternation in the long-chain carotenoids modulated by the dynamical protein environment is a novel finding explaining the high color tunability in crustacyanin.

    Supporting Information

    ARTICLE SECTIONS
    Jump To

    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpclett.8b00763.

    • Details of the approach employed to include the effect of the polarizable environment on the electronic excitation; test calculations for the ωB97X DFT functional and details about the QM/MM BOMD; ωB97X DFT NTOs of AXT; test calculations on the effect of the basis set and the polarizable FF (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 24 publications.

    1. Matteo Ambrosetti, Sulejman Skoko, Tommaso Giovannini, Chiara Cappelli. Quantum Mechanics/Fluctuating Charge Protocol to Compute Solvatochromic Shifts. Journal of Chemical Theory and Computation 2021, 17 (11) , 7146-7156. https://doi.org/10.1021/acs.jctc.1c00763
    2. Jógvan Magnus Haugaard Olsen, Viacheslav Bolnykh, Simone Meloni, Emiliano Ippoliti, Martin P. Bircher, Paolo Carloni, Ursula Rothlisberger. MiMiC: A Novel Framework for Multiscale Modeling in Computational Chemistry. Journal of Chemical Theory and Computation 2019, 15 (6) , 3810-3823. https://doi.org/10.1021/acs.jctc.9b00093
    3. Marius Hervé, Richard Brédy, Gabriel Karras, Bruno Concina, Jeffery Brown, Abdul-Rahman Allouche, Franck Lépine, Isabelle Compagnon. On-the-Fly Femtosecond Action Spectroscopy of Charged Cyanine Dyes: Electronic Structure versus Geometry. The Journal of Physical Chemistry Letters 2019, 10 (9) , 2300-2305. https://doi.org/10.1021/acs.jpclett.9b00435
    4. Andrew Wildman, Greta Donati, Filippo Lipparini, Benedetta Mennucci, Xiaosong Li. Nonequilibrium Environment Dynamics in a Frequency-Dependent Polarizable Embedding Model. Journal of Chemical Theory and Computation 2019, 15 (1) , 43-51. https://doi.org/10.1021/acs.jctc.8b00836
    5. Shinji Kawasaki, Takayuki Kaneko, Tomomi Asano, Takashi Maoka, Shinichi Takaichi, Yasuhito Shomura. An ependymin-related blue carotenoprotein decorates marine blue sponge. Journal of Biological Chemistry 2023, 299 (9) , 105110. https://doi.org/10.1016/j.jbc.2023.105110
    6. Emrah Özcan, Valentyna Kuznetsova, Gürkan Keşan, Marcel Fuciman, Radek Litvín, Tomáš Polívka. Ultrafast excited states dynamics of metal ion complexes of the carotenoid astaxanthin. Journal of Photochemistry and Photobiology A: Chemistry 2023, 441 , 114737. https://doi.org/10.1016/j.jphotochem.2023.114737
    7. Jun Wang, Bo Durbeej. Thermal Fluctuations in Conjugation and their Effect on Calculated Excitation Energies: A Case Study on the Astaxanthin Carotenoid. ChemPhotoChem 2022, 6 (1) https://doi.org/10.1002/cptc.202100178
    8. Florent Figon, Jérôme Casas. The Integrative Biology of Pigment Organelles, a Quantum Chemical Approach. Integrative and Comparative Biology 2021, 61 (4) , 1490-1501. https://doi.org/10.1093/icb/icab045
    9. Canyi Yu, Xiaorong Wang, Yang Wang, Dongjian Shi, Weifu Dong, Lan Zhou, Guojin Liu, Hongji Zhang. Patternable structural color prepared by using photonic crystal paints with high solid content. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2021, 627 , 127212. https://doi.org/10.1016/j.colsurfa.2021.127212
    10. Yigal Lahav, Dror Noy, Igor Schapiro. Spectral tuning of chlorophylls in proteins – electrostatics vs. ring deformation. Physical Chemistry Chemical Physics 2021, 23 (11) , 6544-6551. https://doi.org/10.1039/D0CP06582J
    11. Sayan Maity, Vangelis Daskalakis, Marcus Elstner, Ulrich Kleinekathöfer. Multiscale QM/MM molecular dynamics simulations of the trimeric major light-harvesting complex II. Physical Chemistry Chemical Physics 2021, 450 https://doi.org/10.1039/D1CP01011E
    12. V. A. Pomogaev, P. N. Kluev, R. R. Ramazanov, A. I. Kononov. Combined Quantum-Classical Simulation of Photoinduced Electronic Density Redistribution from Biopolymer Segments to Photochromic Probes. Russian Physics Journal 2020, 63 (8) , 1386-1394. https://doi.org/10.1007/s11182-020-02182-5
    13. Fran Nekvapil, Simona Cintă Pinzaru, Lucian Barbu–Tudoran, Maria Suciu, Branko Glamuzina, Tudor Tamaș, Vasile Chiș. Color-specific porosity in double pigmented natural 3d-nanoarchitectures of blue crab shell. Scientific Reports 2020, 10 (1) https://doi.org/10.1038/s41598-020-60031-4
    14. Yu Wu, Guojin Liu, Hui Li, Penshuai Han, Jinyu Cheng, Lan Zhou. Preparation and Application of Photonic Crystal Paints with Tunable Structural Colors. physica status solidi (a) 2020, 217 (9) https://doi.org/10.1002/pssa.201900539
    15. František Adamec, Domenica Farci, David Bína, Radek Litvín, Tuhin Khan, Marcel Fuciman, Dario Piano, Tomáš Polívka. Photophysics of deinoxanthin, the keto-carotenoid bound to the main S-layer unit of Deinococcus radiodurans. Photochemical & Photobiological Sciences 2020, 19 (4) , 495-503. https://doi.org/10.1039/D0PP00031K
    16. František Adamec, Domenica Farci, David Bína, Radek Litvín, Tuhin Khan, Marcel Fuciman, Dario Piano, Tomáš Polívka. Photophysics of deinoxanthin, the keto-carotenoid bound to the main S-layer unit of Deinococcus radiodurans. Photochemical & Photobiological Sciences 2020, 19 (4) , 495-503. https://doi.org/10.1039/d0pp00031k
    17. Viacheslav Bolnykh, Jógvan Magnus Haugaard Olsen, Simone Meloni, Martin P. Bircher, Emiliano Ippoliti, Paolo Carloni, Ursula Rothlisberger. MiMiC: Multiscale Modeling in Computational Chemistry. Frontiers in Molecular Biosciences 2020, 7 https://doi.org/10.3389/fmolb.2020.00045
    18. Hangke Ma, Jinqiu Sun, Wanyuan Xu, Wei Gao, Guangwei Hu, Xiaofang Lai, Binlun Yan, Huan Gao. Cloning and functional study of lipocalin: retinol-binding protein-like gene family of the ridgetail white prawn, Exopalaemon carinicauda. Molecular Genetics and Genomics 2020, 295 (2) , 453-464. https://doi.org/10.1007/s00438-019-01633-0
    19. Tommaso Giovannini, Rosario Roberto Riso, Matteo Ambrosetti, Alessandra Puglisi, Chiara Cappelli. Electronic transitions for a fully polarizable QM/MM approach based on fluctuating charges and fluctuating dipoles: Linear and corrected linear response regimes. The Journal of Chemical Physics 2019, 151 (17) https://doi.org/10.1063/1.5121396
    20. Tiejun Wei, Vytautas Balevičius, Tomás Polívka, Alexander V. Ruban, Christopher D. P. Duffy. How carotenoid distortions may determine optical properties: lessons from the Orange Carotenoid Protein. Physical Chemistry Chemical Physics 2019, 21 (41) , 23187-23197. https://doi.org/10.1039/C9CP03574E
    21. Ingo Schelter, Johannes M. Foerster, Alastair T. Gardiner, Aleksander W. Roszak, Richard J. Cogdell, G. Matthias Ullmann, Thiago Branquinho de Queiroz, Stephan Kümmel. Assessing density functional theory in real-time and real-space as a tool for studying bacteriochlorophylls and the light-harvesting complex 2. The Journal of Chemical Physics 2019, 151 (13) https://doi.org/10.1063/1.5116779
    22. Zhifeng Jing, Chengwen Liu, Sara Y. Cheng, Rui Qi, Brandon D. Walker, Jean-Philip Piquemal, Pengyu Ren. Polarizable Force Fields for Biomolecular Simulations: Recent Advances and Applications. Annual Review of Biophysics 2019, 48 (1) , 371-394. https://doi.org/10.1146/annurev-biophys-070317-033349
    23. Maria Agustina Dominguez-Martin, Tomáš Polívka, Markus Sutter, Bryan Ferlez, Sigal Lechno-Yossef, Beronda L. Montgomery, Cheryl A. Kerfeld. Structural and spectroscopic characterization of HCP2. Biochimica et Biophysica Acta (BBA) - Bioenergetics 2019, 1860 (5) , 414-424. https://doi.org/10.1016/j.bbabio.2019.03.004
    24. Tommaso Giovannini, Piero Lafiosca, Balasubramanian Chandramouli, Vincenzo Barone, Chiara Cappelli. Effective yet reliable computation of hyperfine coupling constants in solution by a QM/MM approach: Interplay between electrostatics and non-electrostatic effects. The Journal of Chemical Physics 2019, 150 (12) https://doi.org/10.1063/1.5080810
    Download PDF

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    You’ve supercharged your research process with ACS and Mendeley!

    STEP 1:
    Click to create an ACS ID

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    MENDELEY PAIRING EXPIRED
    Your Mendeley pairing has expired. Please reconnect