uu.seUppsala University Publications
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Spectral Variability in Phycocyanin Cryptophyte Antenna Complexes is Controlled by Changes in the alpha-Polypeptide Chains
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Biochemistry. Univ Barcelona, Fac Pharm & Food Sci, Dept Pharm & Pharmaceut Technol & Phys Chem, Av Joan XXIII S-N, E-08028 Barcelona, Spain;Univ Barcelona, Fac Pharm & Food Sci, Inst Theoret & Computat Chem IQTC UB, Av Joan XXIII S-N, E-08028 Barcelona, Spain.
Univ Pisa, Dipartimento Chim & Chim Ind, Via Risorgimento 35, I-56126 Pisa, Italy;Barcelona Inst Sci & Technol, Inst Res Biomed IRB Barcelona, Baldiri Reixac 10, Barcelona 08028, Spain.ORCID iD: 0000-0003-0848-2908
Univ Pisa, Dipartimento Chim & Chim Ind, Via Risorgimento 35, I-56126 Pisa, Italy.
Princeton Univ, Dept Chem, Washington Rd, Princeton, NJ 08544 USA.
Show others and affiliations
2019 (English)In: CHEMPHOTOCHEM, ISSN 2367-0932, Vol. 3, no 9, p. 945-956Article in journal (Refereed) Published
Abstract [en]

Quantitative models of light harvesting in photosynthetic antenna complexes depend sensitively on the challenging determination of the relative site energies of the pigments. Herein we analyze the basis of the light harvesting properties of four antennae from cryptophyte algae, phycocyanines PC577, PC612, PC630 and PC645, by comparing two alternative theoretical strategies to derive the excitonic Hamiltonian. The first is based on molecular dynamics simulations and subsequent polarizable quantum/molecular mechanics (QM/MMPol) calculations, whereas the second is based on three-layer QM/MMPol/ddCOSMO calculations performed on optimized geometries of the pigments, where the water solvent is described using the ddCOSMO continuum model. We find the latter approach to be remarkably accurate, suggesting that these four phycobiliproteins share a common energetic ordering PCB82 < PCB158 < DBV51/61 for pigments located in the highly-conserved beta chains, whereas bilins in the more divergent alpha chains cause their spectral differences. In addition, we predict a strong screening of the coupling among central dihydrobiliverdins (DBVs) in "open" form complexes PC577 and PC612 compared to "closed" form ones, which together with the increased interpigment separation explains the attenuation of coherence beatings observed for these complexes.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH , 2019. Vol. 3, no 9, p. 945-956
Keywords [en]
computational photochemistry, energy transfer, photosynthesis, phycobiliproteins, pigment-protein complexes, QM, MM
National Category
Biochemistry and Molecular Biology
Identifiers
URN: urn:nbn:se:uu:diva-395699DOI: 10.1002/cptc.201900045ISI: 000487014600031OAI: oai:DiVA.org:uu-395699DiVA, id: diva2:1365067
Available from: 2019-10-23 Created: 2019-10-23 Last updated: 2019-10-23Bibliographically approved

Open Access in DiVA

No full text in DiVA

Other links

Publisher's full text

Search in DiVA

By author/editor
Corbella, MarinaCupellini, Lorenzo
By organisation
Biochemistry
Biochemistry and Molecular Biology

Search outside of DiVA

GoogleGoogle Scholar

doi
urn-nbn

Altmetric score

doi
urn-nbn
Total: 36 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf