Dynamics of photoexcitation and stimulated optical emission in conjugated polymers: A multiscale quantum-chemistry and Maxwell-Bloch-equations approach

Stefan Schumacher, Ian Galbraith, Arvydas Ruseckas, Graham A. Turnbull, Ifor D. W. Samuel

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13 Citations (Scopus)

Abstract

We present a general microscopic theory of intense optical pulse propagation in conjugated polymers. The multiscale theory is based on a combination of density-functional theory on the molecular level and many-particle vibronic density matrices which act as a source in Maxwell's equations. The resulting equations are solved nonperturbatively in the light field to study optical amplification and lasing. We illustrate our approach using a polyfluorene material of particular current interest containing a small component of planar (beta-phase) chromophores. Significant reshaping of amplified light pulses is found, stemming from the interplay between light propagation and the excitation of numerous vibrational modes. Furthermore a rich dynamic is observed in the amplified spontaneous emission regime with oscillatory structures rooted in the dynamical population and depopulation of lattice modes.

Original languageEnglish
Article number245407
Number of pages11
JournalPhysical Review. B, Condensed matter and materials physics
Volume81
Issue number24
DOIs
Publication statusPublished - 4 Jun 2010

Keywords

  • BETA-PHASE
  • SEMICONDUCTOR MICROCAVITIES
  • NONLINEAR OPTICS
  • LIGHT
  • SPECTRA
  • SYSTEM
  • STATES
  • GAIN
  • POLY(9,9-DIOCTYLFLUORENE)
  • OLIGOFLUORENES

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