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  1. 1. Principles of charge separator design for artificial photosynthesis 0 | 14Principles of charge separator design for artificial photosynthesis Thomas J. Eisenmayer Universiteit Leiden Leiden Institute of Chemistry.
  2. 2. Principles of charge separator design for artificial photosynthesisIntroduction 1 | 14100% quantumefficiency Leiden Institute of Chemistry.
  3. 3. Principles of charge separator design for artificial photosynthesisIntroduction 1 | 14 Leiden Institute of Chemistry.
  4. 4. Principles of charge separator design for artificial photosynthesisAnisotropic electron transfer 2 | 14 Leiden Institute of Chemistry.
  5. 5. Principles of charge separator design for artificial photosynthesisAnisotropic electron transfer 2 | 14 • Coupled to well-defined vibrational coherences Leiden Institute of Chemistry.
  6. 6. Principles of charge separator design for artificial photosynthesisModel and methods 3 | 14The Special Pair AIMD d 2 Ri Mi =− i Ψ0 | He |Ψ0 dt 2 He Ψ0 = E0 Ψ0 ROKS E (S1 ) = 2E (m) − E (t) Leiden Institute of Chemistry.
  7. 7. Principles of charge separator design for artificial photosynthesisFrontier orbital localization 4 | 14 • HOMO • LUMO + − − + |PL PM |P ∗ |PL PM Leiden Institute of Chemistry.
  8. 8. Principles of charge separator design for artificial photosynthesisFrontier orbital localization 4 | 14 • HOMO • LUMO + − − + |PL PM |P ∗ |PL PM Leiden Institute of Chemistry.
  9. 9. Principles of charge separator design for artificial photosynthesisFrontier orbital localization 4 | 14 • HOMO • LUMO + − − + |PL PM |P ∗ |PL PM Leiden Institute of Chemistry.
  10. 10. Principles of charge separator design for artificial photosynthesisFrontier orbital localization 4 | 14 • HOMO • LUMO + − − + |PL PM |P ∗ |PL PM Leiden Institute of Chemistry.
  11. 11. Principles of charge separator design for artificial photosynthesisLow-frequency vibrational modes 5 | 14 Leiden Institute of Chemistry.
  12. 12. Principles of charge separator design for artificial photosynthesisAnisotropic charge displacement 6 | 14 T.J. Eisenmayer et al., J. Phys. Chem. Lett, 2012, 3 (6), pp 694-697 Leiden Institute of Chemistry.
  13. 13. Principles of charge separator design for artificial photosynthesisWeakening of a hydrogen bond 7 | 14...prevents the back-reaction Leiden Institute of Chemistry.
  14. 14. Principles of charge separator design for artificial photosynthesisModel and methods 8 | 14Including the acceptor CDFT w(r )ρ(r )d (r ) − Nc = 0 AIMD d 2 Ri Mi =− i Ψ0 | He |Ψ0 dt 2 He Ψ0 = E0 Ψ0 Leiden Institute of Chemistry.
  15. 15. Principles of charge separator design for artificial photosynthesisWater A as a ± 32 cm−1 switch 9 | 14 Leiden Institute of Chemistry.
  16. 16. Principles of charge separator design for artificial photosynthesisIncreased coupling 10 | 14 • The donor-acceptor electronic coupling increases with 35% along the suggested reaction coordinate Leiden Institute of Chemistry.
  17. 17. Principles of charge separator design for artificial photosynthesisConclusion 11 | 14 • Removing the barrier → HisM202 rotation • Facilitating electron transfer → Collinear proton displacement • Preventing the back-reaction → Orthogonal proton displacement T.J. Eisenmayer, J. Lasave, F. Buda, to be submitted Leiden Institute of Chemistry.
  18. 18. Principles of charge separator design for artificial photosynthesisWhy is the PSII oxidation potential so high? 12 | 14• the HOMO-5 (PD1 ) is • the dielectric constant is low localized ≈2 Leiden Institute of Chemistry.
  19. 19. Principles of charge separator design for artificial photosynthesisTowards artificial photosynthesis 13 | 14 Leiden Institute of Chemistry.
  20. 20. Principles of charge separator design for artificial photosynthesisDonor-acceptor complex 14 | 14future direction: develop a method to calculate the quantum yield for systems of 50-100 atoms. Leiden Institute of Chemistry.
  21. 21. Principles of charge separator design for artificial photosynthesisDonor-acceptor complex 14 | 14future direction: develop a method to calculate the quantum yield for systems of 50-100 atoms. Leiden Institute of Chemistry.
  22. 22. Principles of charge separator design for artificial photosynthesisDonor-acceptor complex 14 | 14future direction: develop a method to calculate the quantum yield for systems of 50-100 atoms. Leiden Institute of Chemistry.
  23. 23. Principles of charge separator design for artificial photosynthesisDonor-acceptor complex 14 | 14future direction: develop a method to calculate the quantum yield for systems of 50-100 atoms. Leiden Institute of Chemistry.
  24. 24. Principles of charge separator design for artificial photosynthesisAcknowledgements 14 | 14 • Francesco Buda • Jeroen Rombouts (VU) • Huub J.M. de Groot • Adriano Monti • Johannes Neugebauer • Elbert van de Wetering (TU Braunschweig) • Huub Adriaanse • Jorge Lasave (Conicet) • Nitin Bughwansing Leiden Institute of Chemistry.

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