Abstract

New synthesis techniques for highly concentrated colloidal ${\mathrm{C}}_{60}$ suspensions were developed. The nonlinear absorption and nonlinear scattering behavior of colloidal ${\mathrm{C}}_{60}$ suspensions and benchmark materials (carbon black suspension and ${\mathrm{C}}_{60}$ 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 ${\mathrm{C}}_{60}$ 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. ${\mathrm{C}}_{60}$ 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 ${\mathrm{C}}_{60}$ colloids, stronger nonlinear absorption response was found to diminish the nonlinear scattering response. Large, crystalline ${\mathrm{C}}_{60}$ colloids had a stronger nonlinear optical response than benchmarks.

© 2013 Optical Society of America

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