Abstract
The switching of second-harmonic generation (SHG) at a C60 single-crystal surface has been observed in a pump-and-probe experiment. The SHG signal from a picosecond 1.17 eV laser pulse is suppressed by one order of magnitude upon illuminating the crystal surface with a 3.49 eV pump pulse. The nonlinear optical response is faster than 45 ps and persists for longer than 20 ns. SHG suppression to 1/e occurs at pump densities as low as 2.8 μJ/cm2. We suggest that nonlocalized excited electronic states determine the change in the nonlinear optical behavior.
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