Journal of Chemical Physics
Feedback | Help | Exit
The Journal of Chemical Physics
Search:
   
 
 
 
Previous Article
Lithium ion insertion in nanoporous anatase TiO2 studied with RIXS
Lithium insertion into nanoporous anatase TiO2 electrodes has been studied using resonant inelastic soft-x-ray scattering spectroscopy (RIXS). We have measured Ti 2p absorption, L2,3-emission and reso...
Next Article
Statistical thermodynamics of polymer solutions
The previous theory of pure polymer fluid is extended to polymer solutions. The partition function and the complete thermodynamic description for polymer solutions on a lattice model are obtained. Wit...

Dissipative dynamics of spin-dependent electron–hole capture in conjugated polymers

J. Chem. Phys. 119, 3988 (2003); doi:10.1063/1.1591719

Issue Date: 15 August 2003

You are not logged in to this journal. Log in

Stoyan Karabunarliev and Eric R. Bittner
Department of Chemistry and Center for Materials Chemistry, University of Houston, Houston, Texas 77204-5003
Spin-dependent electron–hole (e–h) recombination in poly(p-phenylenevinylene) chains is modeled by the dissipative dynamics of the multilevel electronic system coupled to the phonon bath. The underlying Hamiltonian incorporates the Coulomb and exchange interactions of spin-singlet and spin-triplet monoexcitations in Wannier-orbital basis and their coupling to the prominent Franck–Condon active modes. In agreement with experiment, we obtain that the ratio of singlet versus triplet exciton formation rates is strongly conjugation-length dependent and increasing on going from the model dimer to the extended chain. The result is rationalized in terms of a cascade interconversion mechanism across the electronic levels. In parallel to the direct formation of spin-dependent excitons, e–h capture is found to generate long-lived charge-transfer states, whose further phonon-mediated relaxation to the bottom of the density of states is hindered by the near e–h symmetry of conjugated hydrocarbons. Being nearly spin independent, such states most likely form an intersystem crossing pre-equilibrium, from which the singlet e–h binding channel is about ten times faster than the triplet one. ©2003 American Institute of Physics.
History: Received 19 February 2003; accepted 21 May 2003
Permalink: http://link.aip.org/link/?JCPSA6/119/3988/1
BUY THIS ARTICLE   (US$24)
Download HTML Download Sectioned HTML Download PDF (416 kB) View Cart

KEYWORDS and PACS

Keywords
PACS
  • 72.80.Le
    Electrical conductivity of polymers; organic compounds including organic semiconductors
  • 72.15.Nj
    Collective modes (e.g., in one-dimensional conductors) including synthetic metals
  • YEAR: 2003

RELATED DATABASES


To view database links for this article,
you need to log in.
To view database links for this article,
you need to log in.

PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
Publisher:
AIP is a member of CrossRef AIP

REFERENCES (51)
View in Separate Window/Tab
For access to fully linked references, you need to log in. For access to fully linked references, you need to Log in.
  1. For a review, see R. H. Friend et al., Nature (London) 397, 121 (1999).
  2. A. Kohler, J. S. Wilson, and R. H. Friend, Adv. Mater. (Weinheim, Ger.) 14, 701 (2002).
  3. D. Hertel, S. Setayesh, H. G. Nothofer, U. Scherf, K. Müllen, and H. Bässler, Adv. Mater. (Weinheim, Ger.) 13, 65 (2001).
  4. Y. Cao, I. D. Parker, G. Yu, C. Zhang, and A. J. Heeger, Nature (London) 397, 414 (1999).
  5. J. S. Kim, P. K. H. Ho, N. C. Greenham, and R. H. Friend, J. Appl. Phys. 88, 1073 (2000).
  6. P. K. H. Ho, J. S. Kim, J. H. Burroughes, H. Becker, S. F. Y. Li, T. M. Brown, F. Cacialli, and R. H. Friend, Nature (London) 404, 481 (2000).
  7. T. W. Hagler, K. Pakbaz, K. F. Voss, and A. J. Heeger, Phys. Rev. B 44, 8652 (1991);
    8. T. W. Hagler, K. Pakbaz, and A. J. Heeger, ibid. 49, 10968 (1994).
  8. C. H. Lee, G. Yu, D. Moses, and A. J. Heeger, Phys. Rev. B 49, 2396 (1994);
    9. C. H. Lee, G. Yu, and A. J. Heeger, ibid. 47, 15543 (1993).
  9. For a review, see M. Wohlgenannt and Z. V. Vardeny, J. Phys. Condens. Matter 15, R83 (2003).
  10. J. L. Bredas, J. Cornil, and A. J. Heeger, Adv. Mater. (Weinheim, Ger.) 8, 447 (1996).
  11. D. Beljonne, Z. Shuai, R. H. Friend, and J. L. Bredas, J. Chem. Phys. 102, 2042 (1995).
  12. J. L. Bredas, J. Cornil, D. Beljonne, D. A. Dos Santos, and Z. G. Shuai, Acc. Chem. Res. 32, 267 (1999).
  13. R. Osterbacka, M. Wohlgenannt, D. Chinn, and Z. V. Vardeny, Phys. Rev. B 60, R11253 (1999).
  14. A. P. Monkman, H. D. Burrows, M. D. Miguel, I. Hamblett, and S. Navaratnam, Chem. Phys. Lett. 307, 303 (1999).
  15. A. P. Monkman, H. D. Burrows, L. J. Hartwell, L. E. Horsburgh, I. Hamblett, and S. Navaratnam, Phys. Rev. Lett. 86, 1358 (2001).
  16. N. Chawdhury, et al., J. Chem. Phys. 110, 4963 (1999).
  17. J. S. Wilson, N. Chawdhury, M. R. A. Al-Mandhary, M. Younus, M. S. Khan, P. R. Raithby, A. Kohler, and R. H. Friend, J. Am. Chem. Soc. 123, 9412 (2001).
  18. V. Dyakonov and E. L. Frankevich, Chem. Phys. 227, 203 (1998).
  19. A. S. Dhoot, D. S. Ginger, D. Beljonne, Z. Shuai, and N. C. Greenham, Chem. Phys. Lett. 360, 195 (2002).
  20. J. Partee, E. L. Frankevich, B. Uhlhorn, J. Shinar, Y. Ding, and T. J. Barton, Phys. Rev. Lett. 82, 3673 (1999).
  21. M. Wohlgenannt, K. Tandon, S. Mazumdar, S. Ramasesha, and Z. V. Vardeny, Nature (London) 409, 494 (2001).
  22. Z. G. Soos, S. Ramasesha, and D. S. Galvao, Phys. Rev. Lett. 71, 1609 (1993).
  23. J. S. Wilson, A. S. Dhoot, A. J. A. B. Seeley, M. S. Khan, A. Kohler, and R. H. Friend, Nature (London) 413, 828 (2001).
  24. M. Wohlgenannt, X. M. Jiang, Z. V. Vardeny, and R. A. J. Janssen, Phys. Rev. Lett. 88, 197401 (2002).
  25. M. N. Kobrak and E. R. Bittner, Phys. Rev. B 62, 11473 (2000).
  26. D. Beljonne, Z. Shuai, J. Cornil, J. P. Calbert, and J. L. Bredas, J. Photochem. Photobiol., A 144, 57 (2001);
    27. D. Beljonne (private communication).
  27. Z. Shuai, D. Beljonne, R. J. Silbey, and J. L. Bredas, Phys. Rev. Lett. 84, 131 (2000).
  28. A. Ye, Z. Shuai, and J. L. Bredas, Phys. Rev. B 65, 045208 (2002).
  29. K. Tandon, S. Ramasesha, and S. Mazumdar, Phys. Rev. B 67, 045109 (2003).
  30. M. Y. Lavrentiev, W. Barford, S. J. Martin, H. Daly, and R. J. Bursill, Phys. Rev. B 59, 9987 (1999).
  31. S. Karabunarliev and E. R. Bittner, J. Chem. Phys. 118, 4291 (2003).
  32. S. Karabunarliev and E. R. Bittner, Phys. Rev. Lett. 90, 057402 (2003).
  33. P. Karadakov, J. L. Calais, and J. Delhalle, J. Chem. Phys. 94, 8520 (1991).
  34. D. Mukhopadhyay, G. W. Hayden, and Z. G. Soos, Phys. Rev. B 51, 9476 (1995).
  35. M. Chandross, Y. Shimoi, and S. Mazumdar, Phys. Rev. B 59, 4822 (1999).
  36. N. Marzari and D. Vanderbilt, Phys. Rev. B 56, 12847 (1997), and references therein.
  37. K. Pichler, D. A. Halliday, D. D. C. Bradley, P. L. Burn, R. H. Friend, and A. B. Holmes, J. Phys.: Condens. Matter 5, 7155 (1993).
  38. J. Cornil, D. Beljonne, C. M. Heller, I. H. Campbell, B. K. Laurich, D. L. Smith, D. D. C. Bradley, K. Müllen, and J. L. Bredas, Chem. Phys. Lett. 278, 139 (1997).
  39. G. Mao, J. E. Fischer, F. E. Karasz, and M. J. Winokur, J. Chem. Phys. 98, 712 (1993).
  40. S. Karabunarliev, M. Baumgarten, E. R. Bittner, and K. Müllen, J. Chem. Phys. 113, 11372 (2000).
  41. For a recent review see: V. May and O. Kühn, Charge and Energy Transfer Dynamics in Molecular Systems (Wiley, Berlin, 2000).
  42. W. T. Pollard and R. A. Friesner, J. Chem. Phys. 100, 5054 (1994), and references therein.
  43. R. Kersting, U. Lemmer, R. F. Mahrt, K. Leo, H. Kurz, H. Bässler, and O. E. Göbel, Phys. Rev. Lett. 70, 3820 (1993);
    44. R. Kersting, U. Lemmer, M. Deussen, H. J. Bakker, R. F. Mahrt, H. Kurz, V. I. Arkhipov, H. Bässler, and O. E. Göbel, ibid. 73, 1440 (1994).
  44. V. I. Arkhipov, E. V. Emelianova, and H. Bässler, Phys. Rev. Lett. 82, 1321 (1999);
    45. V. I. Arkhipov, E. V. Emelianova, S. Barth, and H. Bässler, Phys. Rev. B 61, 8207 (2000).
  45. S. H. Lim, T. G. Bjorklund, and C. J. Bardeen, Chem. Phys. Lett. 342, 555 (2001).
  46. It is shown in Ref. 31 that the bipolaron stabilization of both SXT and TXT is about 0.2 eV. It does not affect substantially the singlet–triplet difference and the average e–h separations in the wave functions.
  47. A. Kohler, D. A. Dos Santos, D. Beljonne, Z. Shuai, J. L. Bredas, A. B. Holmes, A. Kraus, K. Müllen, and R. H. Friend, Nature (London) 392, 903 (1998).
  48. S. V. Frolov, Z. Bao, W. Wohlgenannt, and Z. V. Vardeny, Phys. Rev. B 65, 205209 (2001).
  49. CT population values are also corrected for the presence of thermally accessible odd e–h parity states.
  50. A. R. Brown, K. Pichler, N. C. Greenham, D. D. C. Bradley, R. H. Friend, and A. B. Holmes, Chem. Phys. Lett. 210, 61 (1993).
  51. A. L. Burin and M. A. Ratner, J. Chem. Phys. 109, 6092 (1998).

CITING ARTICLES
For access to citing articles, you need to log in.
For access to citing articles, you need to Log in.


Copyright © American Institute of Physics