Self-sustained pulsation of amplified spontaneous emission of molecules in solution

Abstract

Temporal oscillations of amplified spontaneous emission of molecules are studied theoretically. From the proposed theory and numerical simulations, it is found that the self-pulsations originate in an interplay between stimulated emission and saturable absorption. A stability analysis demonstrates the crucial role of the photoabsorption in this process, which can be regulated by a proper choice of buffer molecules. Variations in the saturable absorption mediate a transition from damped oscillations to self-sustained pulsations. The role of propagation effects as well as of the interaction of co- and counter-propagating pulses is also investigated. Numerical simulations, demonstrating the theoretical findings, are performed for a model 3-level system and for an organic chromophore; 4-[N-(2-hydroxyethyl)-N-(methyl)amino phenyl]-4′-(6-hydroxyhexyl sulphonyl) stilbene.