Quantum coherence controls the charge separation in a prototypical artificial light-harvesting system

Nature Communications

Volumn 4, Issue , 2013, Pages

  Andrea Rozzi, Carlo ^a   Maria Falke, Sarah ^b   Spallanzani, Nicola ^a,c   Rubio, Angel ^d,e   Molinari, Elisa ^a,c   Brida, Daniele ^f   Maiuri, Margherita ^f   Cerullo, Giulio ^f   Schramm, Heiko ^b   Christoffers, Jens ^b   Lienau, Christoph ^b  

^a CNR   (Italy)

^b UNIVERSITY OF OLDENBURG   (Germany)

^c UNIVERSITY OF MODENA AND REGGIO EMILIA   (Italy)

^d UNIVERSITY OF THE BASQUE COUNTRY UPV EHU   (Spain)

^e FRITZ HABER INSTITUT DER MAX PLANCK GESELLSCHAFT   (Germany)

^f POLITECNICO DI MILANO   (Italy)

Author keywords

[No Author keywords available]

Indexed keywords

ELECTRON; LIGHT AVAILABILITY; PHOTOVOLTAIC SYSTEM; QUANTUM MECHANICS; SEPARATION; TIMESCALE;

ARTICLE; CHROMATOPHORE; ELECTRICITY; ELECTROCHEMISTRY; ELECTRON; ELECTRON TRANSPORT; FEMTOSECOND LASER; LIGHT HARVESTING SYSTEM; QUANTUM COHERENCE; SPECTROSCOPY; WAVEFORM;

EID: 84875910871     PISSN: None     EISSN: 20411723     Source Type: Journal    
DOI: 10.1038/ncomms2603     Document Type: Article

References (45)

1. Scholes, G. D., Fleming, G. R., Olaya-Castro, A. & van Grondelle, R. Lessons from nature about solar light harvesting. Nat. Chem. 3, 763-774 (2011).
2. Blankenship, R. E. et al. Comparing photosynthetic and photovoltaic efficiencies and recognizing the potential for improvement. Science 332, 805-809 (2011).
3. Gratzel, M. Photoelectrochemical cells. Nature 414, 338-344 (2001). (Pubitemid 33097816)
4. Brabec, C. J., Sariciftci, N. S. & Hummelen, J. C. Plastic solar cells. Adv. Funct. Mater. 11, 15-26 (2001). (Pubitemid 33046405)
5. Huynh, W. U., Dittmer, J. J. & Alivisatos, A. P. Hybrid nanorod-polymer solar cells. Science 295, 2425-2427 (2002). (Pubitemid 34270250)
6. Engel, G. S. et al. Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems. Nature 446, 782-786 (2007). (Pubitemid 46582029)
7. Collini, E. et al. Coherently wired light-harvesting in photosynthetic marine algae at ambient temperature. Nature 463, 644-647 (2010).
8. Ishizaki, A. & Fleming, G. R. Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature. Proc. Natl Acad. Sci. USA 106, 17255-17260 (2009).
9. Abramavicius, D. & Mukamel, S. Energy-transfer and charge-separation pathways in the reaction center of photosystem II revealed by coherent two-dimensional optical spectroscopy. J. Chem. Phys. 133, 184501 (2010).
10. Lee, H., Cheng, Y.-C. & Fleming, G. R. Coherence dynamics in photosynthesis: protein protection of excitonic coherence. Science 316, 1462-1465 (2007). (Pubitemid 46906609)
11. Kodis, G., Liddell, P. A., Moore, A. L., Moore, T. A. & Gust, D. Synthesis and photochemistry of a carotene-porphyrin-fullerene model photosynthetic reaction center. J. Phys. Org. Chem. 17, 724-734 (2004).
12. Gust, D., Moore, T. A. & Moore, A. L. Mimicking photosynthetic solar energy transduction. Acc. Chem. Res. 34, 40-48 (2001). (Pubitemid 32066588)
13. Kuciauskas, D. et al. Photoinduced electron transfer in carotenoporphyrinfullerene triads: temperature and solvent effects. J. Phys. Chem. B 104, 4307-4321 (2000).
14. Brabec, C. J. et al. Tracing photoinduced electron transfer process in conjugated polymer/fullerene bulk heterojunctions in real time. Chem. Phys. Lett. 340, 232-236 (2001). (Pubitemid 33628163)
15. Huber, R., Moser, J. E., Gratzel, M. & Wachtveitl, J. Real-time observation of photoinduced adiabatic electron transfer in strongly coupled dye/semiconductor colloidal systems with a 6fs time constant. J. Phys. Chem. B 106, 6494-6499 (2002). (Pubitemid 35281782)
16. Baskin, J. S., Yu, H. Z. & Zewail, A. H. Ultrafast dynamics of porphyrins in the condensed phase: I. Free base tetraphenylporphyrin. J. Phys. Chem. A 106, 9837-9844 (2002). (Pubitemid 35410154)
17. Castro, A. et al. Octopus: a tool for the application of time-dependent density functional theory. Phys. Status Solidi B 243, 2465-2488 (2006). (Pubitemid 44368981)
18. Baruah, T. & Pederson, M. R. DFT calculations on charge-transfer states of a carotenoid-porphyrin-C(60) molecular triad. J. Chem. Theory Comput. 5, 834-843 (2009).
19. Spallanzani, N. et al. Photoexcitation of a light-harvesting supramolecular triad: a time-dependent DFT study. J. Phys. Chem. B 113, 5345-5349 (2009).
20. Starcke, J. H., Wormit, M., Schirmer, J. & Dreuw, A. How much double excitation character do the lowest excited states of linear polyenes have? Chem. Phys. 329, 39-49 (2006).
21. Varsano, D., Marini, A. & Rubio, A. Optical saturation driven by exciton confinement in molecular chains: a time-dependent density-functional theory approach. Phys. Rev. Lett. 101, 133002 (2008).
22. Cerullo, G. et al. Photosynthetic light harvesting by carotenoids: detection of an intermediate excited state. Science 298, 2395-2398 (2002). (Pubitemid 36014214)
23. Wohlleben, W. et al. Pump-deplete-probe spectroscopy and the puzzle of carotenoid dark states. J. Phys. Chem. B 108, 3320-3325 (2004).
24. Polli, D. et al. Broadband pump-probe spectroscopy with sub-10-fs resolution for probing ultrafast internal conversion and coherent phonons in carotenoids. Chem. Phys. 350, 45-55 (2008).
25. Kumar, A. T. N., Rosca, F., Widom, A. & Champion, P. M. Investigations of amplitude and phase excitation profiles in femtosecond coherence spectroscopy. J. Chem. Phys. 114, 701-724 (2001). (Pubitemid 32138505)
26. Sufra, S., Dellepiane, G., Masetti, G. & Zerbi, G. Resonance raman-spectrum of beta-carotene. J. Raman Spectrosc. 6, 267-272 (1977).
27. Polli, D. et al. Conical intersection dynamics of the primary photoisomerization event in vision. Nature 467, 440-443 (2010).
28. Bahr, J. L. et al. Driving force and electronic coupling effects on photoinduced electron transfer in a fullerene-based molecular triad. Photochem. Photobiol. 72, 598 (2000).
29. Marques, M. A. L et al.Time-Dependent Density Functional Theory, Lecture Notes in Physics Vol. 620 (Springer, 2003).
30. Hornung, T., Skenderovich, H. & Motzkus, M. Observation of all-trans-betacarotene wavepacket motion on the electronic ground and excited dark state using degenerate four-wave mixing (DFWM) and pump-DFWM. Chem. Phys. Lett. 402, 283-288 (2005). (Pubitemid 40126589)
31. Marcus, R. A. Electron-transfer reactions in chemistry-theory and experiment. Rev. Mod. Phys. 65, 599-610 (1993).
32. Duncan, W. R. & Prezhdo, O. V. Theoretical studies of photoinduced electron transfer in dye-sensitized TiO(2). Annu. Rev. Phys. Chem. 58, 143-184 (2007). (Pubitemid 46877588)
33. Lee, C. H. & Lindsey, J. S. One-flask synthesis of meso-substituted dipyromethanes and their application in the synthesis of trans-substituted porphyrin building blocks. Tetrahedron 50, 11427-11440 (1994).
34. Boyle, R. W., Bruckner, C., Posakony, J., James, B. R. & Dolphin, D. 5-Phenyldipyrromethane and 5,15-diphenylporphyrin. Org. Synth. 76, 287-293 (1999).
35. Carcel, C. M. et al. Porphyrin architectures tailored for studies of molecular information storage. J. Org. Chem. 69, 6739-6750 (2004). (Pubitemid 39304807)
36. Liddell, P. A. et al. Photoinduced electron transfer in tetrathiafulvaleneporphyrin-fullerene molecular triads. Helv. Chim. Acta 84, 2765-2783 (2001). (Pubitemid 33021572)
37. Tagmatarchis, N. & Prato, M. The addition of Azomethine Ylides to [60]Fullerene leading to fulleropyrrolidines. Synlett 6, 768-779 (2003). (Pubitemid 36577752)
38. Gust, D. et al. Triplet and singlet energy transfer in carotene porphyrin dyads: role of the linkage bonds. J. Am. Chem. Soc. 114, 3590-3603 (1992).
39. Horner, L., Hoffmann, H., Wippel, H. G. & Hassel, G. [Zum Spaltungsverlauf gemischt substituierter Tetraaryl-phosphonium-hydroxide]. Chem. Ber. 91, 52-57 (1958).
40. Manzoni, C., Polli, D. & Cerullo, G. Two-color pump-probe system broadly tunable over the visible and the near infrared with sub-30 fs temporal resolution. Rev. Sci. Instrum. 77, 023103 (2006).
41. Polli, D., Lüer, L. & Cerullo, G. High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics. Rev. Sci. Instrum. 78, 103108 (2007).
42. Genovese, L., Deutsch, T., Neelov, A., Goedecker, S. & Beylkin, G. Efficient solution of Poisson's equation with free boundary conditions. J. Chem. Phys. 125, 074105 (2006).
43. Castro, A., Marques, M. A. L. & Rubio, A. Propagators for the time-dependent Kohn-Sham equations. J. Chem. Phys. 121, 3425-3433 (2004).
44. Alonso, J. et al. Efficient formalism for large-scale ab initio molecular dynamics based on time-dependent density functional theory. Phys. Rev. Lett. 101, 096403 (2008).
45. Andrade, X. et al. Modified Ehrenfest formalism for efficient large-scale ab initio molecular dynamics. J. Chem. Theory Comput. 5, 728-742 (2009).