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In this article, the detailed photoexcitation dynamics which combines nonadiabatic molecular dynamics with electronic transitions shows the occurrence of amplified spontaneous emission (ASE) in conjugated polymers, accompanied by spontaneous electric polarization. The elaborate molecular dynamic process of ultrafast photoexcitation can be described as follows: Continuous external optical pumping (laser of 70 µJ/cm 2 ) not only triggers the appearance of an instantaneous four-level electronic structure but causes population inversion for ASE as well. At the same time, the phonon spectrum of the conjugated polymer changes, and five local infrared lattice vibrational modes form at the two ends, which break the original symmetry in the system and leads to charge accumulation at the ends of the polymer chain without an external electric field. This novel phenomenon gives a brand-new avenue to explain how the lattice vibrations play a role in the evolution of the stimulated emission, which leads to an ultrafast effect in solid conjugated polymers.

Charge Accumulation of Amplified Spontaneous Emission in a Conjugated Polymer Chain and Its Dynamical Phonon Spectra