A multiconfigurational time-dependent Hartree-Fock method for excited electronic states. II. Coulomb interaction effects in single conjugated polymer chains

R. P. Miranda*, A. J. Fisher, L. Stella, A. P. Horsfield

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

14 Citations (Scopus)

Abstract

Conjugated polymers have attracted considerable attention in the last few decades due to their potential for optoelectronic applications. A key step that needs optimisation is charge carrier separation following photoexcitation. To understand better the dynamics of the exciton prior to charge separation, we have performed simulations of the formation and dynamics of localised excitations in single conjugated polymer strands. We use a nonadiabatic molecular dynamics method which allows for the coupled evolution of the nuclear degrees of freedom and of multiconfigurational electronic wavefunctions. We show the relaxation of electron-hole pairs to form excitons and oppositely charged polaron pairs and discuss the modifications to the relaxation process predicted by the inclusion of the Coulomb interaction between the carriers. The issue of charge photogeneration in conjugated polymers in dilute solution is also addressed. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3600404]

Original languageEnglish
Article number244102
Number of pages13
JournalJournal of Chemical Physics
Volume134
Issue number24
DOIs
Publication statusPublished - 28 Jun 2011

Keywords

  • conducting polymers
  • excited states
  • excitons
  • HF calculations
  • molecular dynamics method
  • photoexcitation
  • polarons
  • wave functions
  • PHOTOVOLTAIC CELLS
  • MOLECULAR-DYNAMICS
  • ENERGY-GAP
  • POLYACETYLENE
  • POLYENES
  • DIODES
  • PHOTOEXCITATION
  • HETEROJUNCTIONS
  • DELOCALIZATION
  • TRANSITION

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