Abstract
The nonlinear optical properties, optical limitation, and second- and third-order
nonlinearity in a new class of noncovalently bonded fullerene-porphyrin complexes
are investigated. Quantum-chemical calculations of the optimal geometry, binding
energy, electronic structure, and nonlinear optical properties of donor-acceptor
fullerene-prophyrin complexes are performed. As a result of the formation of a
complex, the second-order molecular polarizability is higher than in porphyrins by
two to three orders of magnitude, depending on the orientation of the molecule, and
the third-order molecular susceptibility two orders of magnitude higher. The
nonlinear absorption in thin films and solutions of the complexes is measured. In
picosecond regimes, absorption saturation at 560nm wavelength is observed for pulse energy density above 0.01J/cm<sup>2</sup>. A model is proposed for the increase of the optical nonlinearity in
complexes as compared with the molecular components.
© 2010 Optical Society of America
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