Reflection of light by anisotropic molecular crystals including exciton-polaritons and spatial dispersion

A theory for the reflection of light by molecular crystals is described, which reproduces the minimum within the reflection band that is observed experimentally. The minimum in reflection is related to the excitation of polaritons in the crystal. The theory involves reformulation of the boundary conditions for electromagnetic waves at the interface between vacuum and material. The material is modeled by a cubic lattice of oriented Lorentz oscillators. By requiring uniformity of gauge of the electromagnetic potential across the interface between vacuum and the dipole lattice, the need for additional boundary conditions is obviated. The frequency separation between the maxima in reflectance on both sides of the minimum allows for the extraction of a plasma frequency. The plasma frequencies extracted from reflection spectra are compared to the plasma frequencies calculated directly from structural data on the crystals and the oscillator strengths of the constituent molecules. A good agreement between extracted and calculated plasma frequency is obtained for a set of 11 dye molecules.