New synthesis techniques for highly concentrated colloidal C60 suspensions were developed. The nonlinear absorption and nonlinear scattering behavior of colloidal C60 suspensions and benchmark materials (carbon black suspension and C60 solution) were studied with an apparatus that simultaneously measured the total scattered and transmitted energy, inferring absorbance. These experimental results were compared to simple thermodynamic and reverse saturable absorption models, as well as a hybridized model proposed for the nonlinear optical behavior of C60 colloids. All samples followed an attenuation pattern in the nonlinear scattering regime that was fit by a single extinction coefficient, indicating that the energy in excess of that required to reach the sublimation threshold does not significantly affect the size of the induced scattering centers. C60 colloids evidenced strong quenching of the first excited singlet band, leading to weak intersystem-crossing to the triplet manifold. The degree of quenching was morphology dependent. Tighter crystalline packing led to stronger quenching. Samples with higher triplet quantum yield evidenced less efficient heating of the particles. Consequently, for otherwise similar C60 colloids, stronger nonlinear absorption response was found to diminish the nonlinear scattering response. Large, crystalline C60 colloids had a stronger nonlinear optical response than benchmarks.
|Number of pages
|Journal of the Optical Society of America B: Optical Physics
|Published - Jan 1 2014
ASJC Scopus subject areas
- Statistical and Nonlinear Physics
- Atomic and Molecular Physics, and Optics