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, I. D W Samuel

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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 (ß -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. © 2010 The American Physical Society.

Original languageEnglish
Article number245407
JournalPhysical Review B: Condensed Matter and Materials Physics
Volume81
Issue number24
DOIs
Publication statusPublished - 4 Jun 2010

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