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Page count: 9

Resonantly enhanced surface second-harmonic generation and sum- frequency generation has been demonstrated on rhodamine 6G coated glass substrates using different excitation geometries. The collinearly excited, doubly-resonant sum-frequency signal is enhanced by more than two orders of magnitude relative to resonantly enhanced second-harmonic generation. For noncollinear excitation, the relative efficiency of nonlinear generation as a function of the angular dependence of the input beams is calculated and compared with experiment.