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Author:

Howard, Ian A. (Howard, Ian A..) | Hodgkiss, Justin M. (Hodgkiss, Justin M..) | Zhang, Xinping (Zhang, Xinping.) (Scholars:张新平) | Kirov, Kiril R. (Kirov, Kiril R..) | Bronstein, Hugo A. (Bronstein, Hugo A..) | Williams, Charlotte K. (Williams, Charlotte K..) | Friend, Richard H. (Friend, Richard H..) | Westenhoff, Sebastian (Westenhoff, Sebastian.) | Greenham, Neil C. (Greenham, Neil C..)

Indexed by:

EI Scopus

Abstract:

Bimolecular interactions between excitations in conjugated polymer thin films are important because they influence the efficiency of many optoelectronic devices that require high excitation densities. Using time - resolved optical spectroscopy, we measure the bimolecular interactions of charges, singlet excitons, and triplet excitons in intimately mixed polyfluorene blends with band-edge offsets optimized for photoinduced electron transfer. Bimolecular charge recombination and triplet - triplet annihilation are negligible, but exciton-charge interactions are efficient. The annihilation of singlet excitons by charges occurs on picosecond time-scales and reaches a rate equivalent to that of charge transfer. Triplet exciton annihilation by charges occurs on nanosecond time-scales. The surprising absence of nongeminate charge recombination is shown to be due to the limited mobility of charge carriers at the heterojunction. Therefore, extremely high densities of charge pairs can be maintained in the blend. The absence of triplet - triplet annihilation is a consequence of restricted triplet diffusion in the blend morphology. We suggest that the rate and nature of bimolecular interactions are determined by the stochastic excitation distribution in the polymer blend and the limited connectivity between the polymer domains. A model based on these assumptions quantitatively explains the effects. Our findings provide a comprehensive framework for understanding bimolecular recombination and annihilation processes in nanostructured materials. © 2010 American Chemical Society.

Keyword:

Heterojunctions Electric charge Morphology Optoelectronic devices Polymer blends Stochastic systems Conjugated polymers Excitons Charge transfer Carrier mobility Polymer films

Author Community:

  • [ 1 ] [Howard, Ian A.]Cavendish Laboratory, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • [ 2 ] [Howard, Ian A.]Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
  • [ 3 ] [Hodgkiss, Justin M.]Cavendish Laboratory, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • [ 4 ] [Hodgkiss, Justin M.]School and Chemical and Physical Sciences, MacDiarmid Institute for Advanced Materials and Nanotechnology, Victoria University of Wellington, P.O. Box 600, Wellington, New Zealand
  • [ 5 ] [Zhang, Xinping]Cavendish Laboratory, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • [ 6 ] [Zhang, Xinping]College of Applied Sciences, Beijing University of Technology, Beijing 100022, China
  • [ 7 ] [Kirov, Kiril R.]Cavendish Laboratory, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • [ 8 ] [Bronstein, Hugo A.]Department of Chemistry, Imperial College London, London SW7 2AZ, United Kingdom
  • [ 9 ] [Williams, Charlotte K.]Department of Chemistry, Imperial College London, London SW7 2AZ, United Kingdom
  • [ 10 ] [Friend, Richard H.]Cavendish Laboratory, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • [ 11 ] [Westenhoff, Sebastian]Cavendish Laboratory, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • [ 12 ] [Westenhoff, Sebastian]Department of Chemistry, Biochemistry and Biophysics, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden
  • [ 13 ] [Greenham, Neil C.]Cavendish Laboratory, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom

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Source :

Journal of the American Chemical Society

ISSN: 0002-7863

Year: 2010

Issue: 1

Volume: 132

Page: 328-335

1 5 . 0 0 0

JCR@2022

ESI Discipline: CHEMISTRY;

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 0

SCOPUS Cited Count: 69

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 4

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