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 language | English |
---|---|
Article number | 245407 |
Journal | Physical Review B: Condensed Matter and Materials Physics |
Volume | 81 |
Issue number | 24 |
DOIs | |
Publication status | Published - 4 Jun 2010 |