In this paper we present a comprehensive theoretical description of molecular spectral converters in the specific context of luminescent solar concentrators (LSCs). The theoretical model is an extension to a three-level system interacting with a solar radiation bath of the standard quantum theory of atomic radiative processes. We derive the equilibrium equations of the conversion process and provide specific examples of application of this principle to the development of solar concentration devices. (C) 2010 Elsevier B.V. All rights reserved.