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  On the Exciton Coupling between Two Chlorophyll Pigments in the Absence of a Protein Environment: Intrinsic Effects Revealed by Theory and Experiment

Milne, B. F., Kjær, C., Houmøller, J., Stockett, M. H., Toker, Y., Rubio, A., et al. (2016). On the Exciton Coupling between Two Chlorophyll Pigments in the Absence of a Protein Environment: Intrinsic Effects Revealed by Theory and Experiment. Angewandte Chemie International Edition, 55(21), 6248-6251. doi:10.1002/anie.201601979.

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anie201601979.pdf (Publisher version), 900KB
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© B. F. Milne et al.

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http://dx.doi.org/10.1002/anie.201601979 (Publisher version)
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 Creators:
Milne, Bruce F.1, Author
Kjær, Christina2, Author
Houmøller, Jørgen2, Author
Stockett, Mark H.2, Author
Toker, Yoni3, Author
Rubio, Angel4, 5, Author           
Nielsen, Steen Brøndsted2, Author
Affiliations:
1CFisUC, Department of Physics, University of Coimbra, Rua Larga, 3004–516 Coimbra, Portugal, ou_persistent22              
2Department of Physics and Astronomy, Aarhus University, Ny Munkegade, DK-8000 Aarhus C, Denmark, ou_persistent22              
3Institute of Nanotechnology and Advanced Materials, Bar-Ilan University, Ramat-Gan 5290002, Israel, ou_persistent22              
4Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2074320              
5Nano-Bio Spectroscopy Group and ETSF, Universidad del País Vasco, CFM CSIC-UPV/EHU-MPC & DIPC, 20018 San Sebastián, Spain, ou_persistent22              

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Free keywords: absorption spectroscopy; chlorophyll; density functional calculations; mass spectrometry; photosynthesis
 Abstract: Exciton coupling between two or more chlorophyll (Chl) pigments is a key mechanism associated with the color tuning of photosynthetic proteins but it is difficult to disentangle this effect from shifts that are due to the protein microenvironment. Herein, we report the formation of the simplest coupled system, the Chl a dimer, tagged with a quaternary ammonium ion by electrospray ionization. Based on action spectroscopic studies in vacuo, the dimer complexes were found to absorb 50–70 meV to the red of the monomers under the same conditions. First-principles calculations predict shifts that somewhat depend on the relative orientation of the two Chl units, namely 50 and 30 meV for structures where the Chl rings are stacked and unstacked, respectively. Our work demonstrates that Chl association alone can produce a large portion of the color shift observed in photosynthetic macromolecular assemblies.

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Language(s): eng - English
 Dates: 2016-02-252016-04-132016-05-17
 Publication Status: Issued
 Pages: 4
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.201601979
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Title: Angewandte Chemie International Edition
  Other : Angewandte Chemie, International Edition
  Abbreviation : Angew. Chem. Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 55 (21) Sequence Number: - Start / End Page: 6248 - 6251 Identifier: ISSN: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851