NONLINEAR LUMINESCENCE PHENOMENA IN FULLERENE CRYSTALLITES

Time-resolved photoluminescence studies in powders and single crystals of C60 are reported. The observed emission spectra, resulting from excitation above the HOMO-LUMO transition energy, are consistent with those reported for steady state conditions which may be associated with an intramolecular process and the observed luminescence decay times are of the order of 1 ns. No long lived decay from the triplet is observed at low intensities. A dramatic increase in the lifetime as well as a redshift and broadening of the spectrum is observed at high excitation densities. The luminescence intensity is seen to increase with the cube of the input intensity. The phenomenon is interpreted as an abrupt onset of emission from the highly populated excited state resulting from an interaction of the intramolecular states, a process which is dependent on a critical excited state density. Furthermore, the phenomenon may be photoexcited at photon energies which lie below the HOMO-LUMO transition energy, under which conditions an intensity dependence of the output luminescence on input to the sixth power is observed. Under ''off-resonant'' conditions the process is interpreted as two-photon assisted nonlinear emission.