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Quantum Beating In Photosynthetic Systems using Noisy Light Darin Ulness Department of Chemistry

Quantum Beating In Photosynthetic Systems using Noisy Light Darin Ulness Department of Chemistry Concordia College, Moorhead, MN. Quantum Beating In Photosynthetic Systems using Noisy Light Darin Ulness Department of Chemistry Concordia College, Moorhead, MN.

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Quantum Beating In Photosynthetic Systems using Noisy Light Darin Ulness Department of Chemistry

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  1. Quantum Beating In Photosynthetic Systems using Noisy Light Darin Ulness Department of Chemistry Concordia College, Moorhead, MN

  2. Quantum Beating In Photosynthetic Systems using Noisy Light Darin Ulness Department of Chemistry Concordia College, Moorhead, MN

  3. Quantum Beating In Photosynthetic Systems using Noisy Light Darin Ulness Department of Chemistry Concordia College, Moorhead, MN

  4. Quantum Biology Magneto-reception Olfactation Enzymes Photosynthesis

  5. Fenna-Matthews-Olson (FMO) Complex Green Sulfur Bacteria

  6. Fenna-Matthews-Olson (FMO) Complex

  7. Energy Transfer Funnel

  8. Incoherent Energy Transfer Forster Resonant Energy Transfer

  9. Incoherent Energy Transfer Forster Resonant Energy Transfer Another route Coherent Energy Transfer Quantum beating

  10. Quantum beating wb P(t) P(t) = ½ + ½cos(wbt) t

  11. Quantum beating wb wb P(t) P(t) = ½ + ½cos(wbt) t

  12. wb Quantum beating…in a bath L

  13. Quantum beating…in a bath wb P(t) L small L L large t

  14. Quantum coupling wb wb J

  15. J = 0 J = small J = large J = med

  16. J = 0 J = large Local Basis Delocalized Basis

  17. J = 0 J = large Local Basis Delocalized Basis

  18. J = 0 J = large Local Basis Delocalized Basis N N N N

  19. J = 0 J = large Local Basis Delocalized Basis N N N N

  20. J = 0 J = large Local Basis Exciton Basis

  21. J = 0 J = med Local Basis Exciton Basis

  22. J Local Basis Exciton Basis Energy t t t t

  23. Coherent Light Phase locked

  24. Incoherent “noisy” Light Color Locked

  25. Time resolution on the order of the correlation time, tc Noisy Light Spectrum Frequency Noisy Light: Definition • Broadband • Phase incoherent • Quasi continuous wave

  26. Sunlight is Noisy Light!

  27. Material Signal Light field P(t) = P(1) + P(2) + P(3) … P(1) = c(1)E, P(2) = c(2)EE, P(3) = c(3)EEE Nonlinear Spectroscopy P= cE Perturbation series approximation

  28. Light source Interferometer A, B, and C beams Local Oscillator (LO) Sample Signal (S beam) Homodyne intensity is observed

  29. k A S λ = ±s or ±t φ = z or k s z B C t

  30. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator

  31. Difficulty • The cw nature requires all field action permutations. The light is always on. • The proper treatment of the noise cross-correlates chromophores. Solution • Factorized time correlation (FTC) diagram analysis Theoretical Challenges • Complicated Mathematics • Complicated Physical Interpretation

  32. Messy integration and algebra Construction Rules Evaluation Rules Set of intensity level terms (pre-evaluated) Set of FTC diagrams Set of evaluated intensity level terms easy Physics hard hard FTC Diagram Analysis

  33. Utility of FTC Diagrams • Organize lengthy calculations • Error checking • Identification of important terms • Immediate information of about features of spectrograms • Much physical insight that transcends the choice of mathematical model.

  34. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S s z B C t

  35. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S s z Timeline for signal B C t Timeline for LO

  36. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S s Field Interactions z Timeline for signal B C t Timeline for LO

  37. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S s Material Response z Timeline for signal B C t Timeline for LO

  38. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S Correlated Field Action s z Timeline for signal B C t Timeline for LO

  39. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S s One Example z Timeline for signal A B C B C t Timeline for LO

  40. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S s One Example z Timeline for signal A B C B C t Timeline for LO

  41. Noisy Light Spectroscopy Optical coherence theory Perturbation theory: Density operator Construction of an FTC Diagram k A S s One Example z Timeline for signal A B C B C t Timeline for LO

  42. FTC diagrams k A S 128 terms = 128 FTC diagrams s z B C t

  43. FTC diagrams FTC diagrams k A S 128 terms = 128 FTC diagrams s z Only 3 topological classes! B C t

  44. Topological classes of FTC Diagrams • Unrestricted • Singly Restricted • Doubly Restricted

  45. Topological classes of FTC Diagrams • Unrestricted • Singly Restricted • Doubly Restricted Strong ! Weak ! Weak !

  46. Analytic Results: Unrestricted Strong Signal No quantum beating

  47. Analytic Results: Singly restricted Weak Signal Quantum beating

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