Optical excitation waves in a molecular crystal

We have used the quantum theory of radiation, within the time-dependent Hartree approximation, to study exciton states of a van der Waals molecular crystal. The radiation variables are eliminated to give a semi-classical picture of molecular dipoles interacting through a retarded potential, and the solutions of the Hartree equations are closely connected with the quasi-particle excited states in Agranovich’s theory. In the Lorentz-Lorenz approximation the crystal has excited states which correspond to both longitudinal and transverse exciton weaves, and the refractive index behaves classically. The paper concludes with a brief discussion of metallic reflexion by dye crystals.