[en] This work focuses on two fundamental processes in organic solar cellsexciton dissociation and charge recombinationand describes how quantum-chemical calculations can be exploited to estimate the molecular parameters that determine the rates of these processes. The general concepts behind our approach are illustrated by considering a donor-acceptor complex made of a phthalocyanine (electron donor) molecule and a perylene (acceptor) molecule. The results highlight how the relative rates of the two processes depend on the dimensionality of the molecules, their relative positions, the symmetry of the relevant electronic levels, and the polarity of the medium. It is shown, for instance, that highly symmetric configurations of the complex can strongly limit charge recombination; this emphasizes the need for a fine control of the supramolecular organization at organic-organic interfaces in donor-acceptor blends.
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.; Lögdlund, M.; Salaneck, W. R. Nature 1999, 397, 121.
Borchardt, J. K. Mater. Today, September 2004, 42.
Sariciftci, N. S.; Smilowitz, L.; Heeger, A. J.; Wudl, F. Science 1992, 58, 1474.
Horowitz, G. Adv. Mater. 1998, 10, 365.
Tessler, N. Adv. Mater. 1999, 11, 363.
McQuade, D. T.; Pullen, A. E.; Swager, T. M. Chem. Rev. 2000, 100, 2537.
Brabec, C. J.; Sariciftci, N. S.; Hummelen, J. C. Adv. Funct. Mater. 2001, 11, 15.
Hill, I. G.; Kahn, A.; Soos, Z. G.; Pascal. R. A. Chem. Phys. Lett. 2000, 327, 181.
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.
Yu, G.; Gao, J.; Hummelen, J. C.; Wudl, F.; Heeger, A. J. Science 1995, 270, 1789.
Tang, C. W. Appl. Phys. Lett. 1986, 48, 183.
Wöhrle, D.; Meissner, D. Adv. Mater. 1991, 3, 129.
Svensson, M.; Zhang, F. L.; Veenstra, S. C.; Verhees, W. J. H.; Hummelen, J. C.; Kroon, J. M.; Inganas, O.; Andersson, M. R. Adv. Mater. 2003, 15, 988.
Halls, J. J. M.; Cornil, J.; dos Santos, D. A.; Silbey, R.; Hwang, D. H.; Holmes, A. B.; Brédas, J. L.; Friend, R. H. Phys. Rev. B 1998, 60, 5721.
Pourtois, P.; Beljonne, D.; Cornil, J.; Ratner, M. A.; Brédas, J. L. J. Am. Chem. Soc. 2002, 124, 4436.
Clayton, A. H. A.; Ghiggino, K. P.; Wilson, G. J.; Paddon-Row, M. N. J. Phys. Chem. 1993, 97, 7962.
Filatov, I.; Larsson, S. Chem. Phys. 2002, 284, 575.
Redmore, N. P.; Rubtsov, I. V.; Therien, M. J. J. Am. Chem. Soc. 2003, 125, 8769.
Weiss, E. A.; Ahrens, M. J.; Sinks, L. E.; Gusev, A. V.; Ratner, M. A.; Wasielewski, M. R. J. Am. Chem. Soc. 2004, 126, 5577.
Tang, C. W. Appl. Phys. Lett. 1986, 48, 183.
Wöhrle, D.; Meissner, D. Adv. Mater. 1991, 3, 129.
Adams, D. M.; Kerimo, J.; Olson, E. J. C.; Zaban, A.; Gregg, B. A.; Barbara, P. F. J. Am. Chem. Soc. 1987, 119, 10608.
Lane, P. A.; Rostalski, J.; Giebeler, C.; Martin, S. J.; Bradley, D. D. C.; Meissner, D. Sol. Energy Mater. Sol. Cells 2000, 63, 3.
Hiromitsu, I.; Murakami, Y.; Ito, T. J. Appl. Phys. 2003, 94, 2434.
Aroca, R.; Del Cano, T.; de Saja, J. A. Chem. Mater. 2003, 15, 38.
Edwards, L.; Gouterman, M. J. Mol. Spectrosc. 1979, 33, 292.
Marcus, R. A. Rev. Mod. Phys. 1993, 65, 599.
Barbara, P. F.; Meyer, T. J.; Ratner, M. A. J. Phys. Chem. 1996, 100, 13148.
Sakanoue, K.; Motoda, M.; Sugimoto, M.; Sakaki, S. J. Phys. Chem. A 1999, 103, 5551.
Coropceanu, V.; Malagoli, M.; da Silva Filho, D. A.; Gruhn, N. E.; Bill, T. G.; Brédas, J. L. Phys. Rev. Lett. 2002, 89, 275503.
Electron Transfer: From Isolated Molecules to Biomolecules; Bixon, M., Jortner, J., Eds.; Advances in Chemical Physics, Vol. 106-107; Wiley: New York, 1999.
Cornil, J.; Beljonne, D.; Shuai, Z.; Hagler, T.; Campbell, I.; Bradley, D. D. C.; Brédas, J. L.; Spangler, C. W.; Müllen, K. Chem. Phys. Lett. 1995, 247, 425.
Dewar, M. J. S.; Zoebisch, E. G.; Healy, E. F.; Stewart, J. J. P. J. Am. Chem. Soc. 1985, 107, 3902.
Ampac 6.55; created by Semichem Inc.: Shawnee, KS, 1997.
Klamt, A.; Schürmann, G. J. Chem. Soc., Perkin Trans. 1993, 2, 799.
Zang, D. Y.; So, F. F.; Forrest, S. R. Appl. Phys. Lett. 1991, 59, 823.
Brocks, G.; van den Brink, J.; Morpurgo, A. F. Phys. Rev. Lett. 2004, 93, 146405.
Tant, J.; Lehmann, M.; De Cupere, V.; Zucchi, G.; Lemaur, V.; Marcq, V.; Burquel, A.; Hennebicq, E.; Gardebien, F.; Lazzaroni, R.; Cornil, J.; Laursen, B. W.; Bjornholm, T.; Geerts, Y., submitted for publication.
van Hal, P. A.; Janssen, R. A. J.; Lanzani, G.; Cerullo, G.; Zavelani-Rossi, M.; De Silvestri, S. Phys. Rev. B 2001, 64, 075206.
Arkhipov, V. I.; Heremans, P.; Bässler, H. Appl. Phys. Lett. 2003, 82, 4605.
Offermans, T.; Meskers, S. C. J.; Janssen, R. A. J. J. Chem. Phys. 2003, 119, 10924.
Morteani, A. C.; Sreearunothai, P.; Herz, L. M.; Friend, R. H.; Silva, C. Phys. Rev. Lett. 2004, 92, 247402.
Brédas, J. L.; Beljonne, D.; Coropceanu, V.; Comil, J. Chem. Rev. 2004, 104, 4971.
Marcus, R. A. J. Chem. Phys. 1965, 43, 679.
Handbook of Chemistry and Physics, 76th ed.; Lide, R. D., Frederikse, H. P. R., Eds.; CRC Press: Boca Raton, FL, 1995.
Madigan, C. F.; Bulovic, V. Phys. Rev. Lett. 2003, 91, 247403.
Cave, R. J.; Newton, M. D. Chem. Phys. Lett. 1996, 249, 15.
Cave, R. J.; Newton, M. D. J. Chem. Phys. 1997, 106, 9213.
Nelsen, S. F.; Newton, M. D. J. Phys. Chem. A 2000, 104, 10023.
Ridley, J.; Zerner, M. C. Theor. Chim. Acta 1973, 32, 111.
Rust, M.; Lappe, J.; Cave, R. J. J. Phys. Chem. A 2002, 106, 3930.
Verhoeven, J. W. Adv. Chem. Phys. 1999, 106, 603.
Cave, R. J.; Newton, M. D.; Kumar, K.; Zimmt, M. B. J. Phys. Chem. 1995, 99, 17501.
Lemaur, V.; da Silva Filho, D. A.; Coropceanu, V.; Lehmann, M.; Geerts, Y.; Piris, J.; Debije, M. G.; van de Craats, A. M.; Senthilkumar, K.; Siebbeles, L. D. A.; Warman, J. M.; Brédas, J. L.; Cornil, J. J. Am. Chem. Soc. 2004, 126, 3271.
