Radiative decay of nonstationary system.

Abstract

When a finite quantum system, say a fluorescent molecule is attached to a bulk surface and excited by a short laser pulse, the decay dynamics of the system is modulated by the surface and the signal is enhanced due to the bulk surface. We have considered the decay dynamics of a model of displaced distorted molecule whose excited potential surface is coupled to a continuum and then this first continuum is in turn coupled to a second continuum. In the short time scale there is a coherent exchange of energy between the system molecule and the first continuum states. In the long time scale the energy of the whole system plus first continuum drains out to the final continuum states. A dendrimer nanocomposite with the gold surface shows an enhanced light emission. This can be qualitatively understood from the model we proposed here. We have numerically studied the various potential parameters of the molecule which can affect the signal. When the potential surfaces are flat, the band structure of the first continuum states along with its initial excitation has some nontrivial effect on the profile of the radiative decay.