[en] Atomistic models based on quantum-chemical calculations are combined with time-resolved spectroscopic investigations to explore the migration of electronic excitations along oligophenylenevinylene-based chiral stacks. It is found that the usual Pauli master equation (PME) approach relying on uncoherent transport between individual chromophores underestimates the excitation diffusion dynamics, monitored here by the time decay of the transient polarization anisotropy. A better agreement to experiment is achieved when accounting for excitation delocalization among acceptor molecules, as implemented in a modified version of the PME model. The same models are applied to study light harvesting and trapping in guest-host systems built from oligomers of different lengths.
Disciplines :
Physics
Author, co-author :
Beljonne, David ; Université de Mons > Faculté des Sciences > Chimie des matériaux nouveaux
Burroughes, J. H.; Bradley, D. D. C.; Brown, A. R.; Marks, R. N.; Friend, R. H.; Burn, P. L.; Holmes, A. B. Nature 1990, 347, 539.
Friend, R. H.; Gymer, R. W.; Holmes, A. B.; Burroughes, J. H.; Marks, R. N.; Taliani, C.; Bradley, D. D. C.; dos Santos, D. A.; Brédas, J.-L.; Lögdlund, M.; Salaneck, W. R. Nature 1999, 397, 121.
Sheats, J. R.; Antoniadis, H.; Hueschen, M.; Leonard, W.; Miller, J.; Moon, R.; Roitman, D.; Stocking, A. Science 1996, 273, 884.
Sirringhaus, H.; Brown, P. J.; Friend, R. H.; Nielsen, M. M.; Bechgaard, K.; Langeveld-Voss, B. M. W.; Spiering, A. J. H.; Janssen, R. A. J.; Meijer, E. W.; Herwig, P.; de Leeuw, D. M. Nature 1999, 401, 685.
Halls, J. J. M.; Walsh, C. A.; Greenham, N. C.; Marseglia, E. A.; Friend, R. H.; Moratti, S. C.; Holmes, A. B. Nature 1995, 376, 498.
Brabec, C. J.; Sariciftci, N. S.; Hummelen, J. C. Adv. Funct. Mater. 2001, 11, 15.
Schindler, F.; Lupton, J. M. Proc. Natl. Acad. Sci. U.S.A. 2004, 101, 14695.
Yu, Z. H.; Barbara, P. F. J. Phys. Chem. B 2004, 108, 11321.
Jonkheijm, P.; Hoeben, F. J. M.; Kleppinger, R.; Van Herrikhuyzen, J.; Schenning, A. P. H. J.; Meijer, E. W. J. Am. Chem. Soc. 2003, 125, 15941.
Meskers, S. C. J.; Hübner, J.; Oestreich, M.; Bässler, H. J. Phys. Chem. B 2001, 105, 9139.
Bässler, H.; Schweitzer, B. Acc. Chem. Res. 1999, 32, 173.
Hoeben, F. J. M.; Herz, L. M.; Daniel, C.; Jonkheijm, P.; Schenning, A. P. H. J.; Silva, C.; Meskers, S. C. J.; Beljonne, D.; Phillips, R. T.; Friend, R. H.; Meijer, E. W. Angew. Chem. 2004, 43, 1976.
Herz, L. M.; Daniel, C.; Hoeben, F. J. M.; Schenning, A. P. H. J.; Meijer, E. W.; Friend, R. H.; Philipps, R. T. Phys. Rev. B 2003, 68, 045203.
May, V.; Kühn, O. Charge and Energy Transfer Dynamics in Molecular Systems; Wiley: Berlin, 2000.
Kenkre, V. M.; Knox, R. S. Phys. Rev. Lett. 1974, 9, 5279.
Schatz, G. C.; Ratner, M. A. Quantum Mechanics in Chemistry; Prentice Hall: Englewood Cliffs, NJ, 1993.
Scholes, G. D. Annu. Rev. Phys. Chem. 2003, 54, 57.
Schenning, A. P. H. J.; Jonkheijm, P.; Peeters, E.; Meijer, E. W. J. Am. Chem. Soc. 2001, 123, 409.
Daniel, C. Ph.D. Thesis, Cambridge, U. K., 2004.
Meskers, S. C. J. et al., to be submitted for publication.
Förster, T. Ann. Phys. 1948, 2, 55.
Förster, T. Discuss. Faraday Soc. 1959, 27, 7.
Förster, T. Pure Appl. Chem. 1970, 24, 443.
Förster, T.; Kasper, K. Z. Elektrochem. 1955, 59, 976.
Marguet, S.; Markovitsi, D.; Millié, P.; Sigal, H.; Kumar, S. J. Phys. Chem. B 1998, 102, 4697.
Karaburnaliev, S.; Bittner, E.; Baumgarten, M. J. Chem. Phys. 2001, 114, 5863.
Wiesenhofer, H.; Zojer, E.; List, E. J. W.; Scherf, U.; Brédas, J. L.; Beljonne, D. Phys. Rev. Lett., submitted for publication.
Spano, F. et al., to be submitted for publication.
Bacchiocchi, C.; Zannoni, C. Chem. Phys. Lett. 1997, 268, 541.
Mayo, S. L.; Olafson, B. D.; Goddard, W. A. J. Phys. Chem. 1990, 94, 8897.
Dewar, M. J. S.; Zoebisch, E. G.; Healy, E. F.; Stewart, J. J. P. J. Am. Chem. Soc. 1995, 107, 3702.
Beijer, F. H.; Kooijman, H.; Spek, A. L.; Sijbesma, R. P.; Meijer, E. W. Angew. Chem. 1998, 37, 75.
Ridley, J.; Zerner, M. C. Theor. Chim. Acta 1973, 32, 111.
Hirata, S.; Nooijen, M.; Bartlett, R. J. Chem. Phys. Lett. 2000, 326, 255.
Shuai, Z.; Brédas, J. L. Phys. Rev. B 2000, 62, 15452.
Hennebicq, E.; Pourtois, G.; Scholes, G. D.; Herz, L. M.; Russell, D. M.; Silva, C.; Setayesh, S.; Grimsdale, A. C.; Müllen, K.; Brédas, J.-L., Beljonne, D. J. Am. Chem. Soc. 2005, 127, 4744.
Muller, J. G.; Lemmer; U.; Raschke, G.; Anni, M.; Scherf, U.; Lupton, J. M.; Feldmann, J. Phys. Rev. Lett. 2003, 91, 267403.
Heimel, G. Daghofer, M.; Gierschner, J.; List, E. J. W.; Grimsdale, A. C.; Müllen, K.; Beljonne, D.; Brédas, J.-L.; Zojer, E. J. Chem. Phys. 2005, 122, 054501.
Jang, S. J.; Newton, M. D.; Silbey, R. J. Phys. Rev. Lett. 2004, 92, 218301.