Optical coherence tomography (OCT) is a non-invasive <i>in vivo</i> biomedical imaging modality capable of three-dimensional
visualization of tissue morphology permitting imaging at high speed and sensitivity. Coherent Anti-
Stokes Raman Scattering (CARS) is a nonlinear spectroscopic technique which provides molecular information
due to a four wave mixing process. In order to extend the performance of OCT towards detecting the molecular
fingerprint of biological samples a combined CARS/OCT setup has been developed that employs only a single
ultrashort pulse Ti:Sapphire laser which enables high axial resolution OCT and simultaneously combined with
a spectral shaper a CARS setup. During first measurements the same area of a sample was imaged twice,
applying OCT and CARS consecutively. OCT was used to perform three-dimensional morphological screening.
Due to CARS additional chemical information could be gained for two dimensions. The spectrum was modified
computer controlled to match the requirements for the generation of a CARS signal whereas for OCT the
unmodified spectrum was applied. Fluids such as dimethylsulfoxide (DMSO) and PBS were compared in a
cuvette to demonstrate the functionality of the multimodal setup. As a biological sample a 100 m thickcr oss
section through a human optic nerve surrounded by sclera was investigated.