Three-dimensional vibrational imaging of a microcrystalline J-aggregate using supercontinuum-based ultra-broadband multiplex coherent anti-stokes Raman scattering microscopy

Vibrational properties of a porphyrin J-aggregate microcrystal have been investigated by ultra-broadband multiplex coherent anti-Stokes Raman scattering (CARS) microspectroscopy using a supercontinuum light source generated from a photonic crystal fiber. Owing to a strong resonance effect due to an excitonic transition, clear spectral and spatial profiles of the CARS signal have been successfully obtained. On the basis of the comparison between the CARS and the fluorescence images, the spatial dependence of the CARS signal can be explained by the spatial inhomogeneity of the excitonic transition energy in the single J-aggregate microcrystal.