Singlet molecular oxygen (a(1)Delta (g)) has been produced and optically de
tected upon two-photon nonlinear excitation of a sensitizer with a focused
laser beam. The experiments were performed using toluene solutions with eit
her a substituted difuranonaphthalene or a substituted distyryl benzene as
the sensitizer. The data indicate that the two-photon absorption cross sect
ions of the difuranonaphthalenes are comparatively large and depend signifi
cantly on the functional groups attached to the chromophore. The time-resol
ved 1270 nm phosphorescence signals used to characterize the production of
singlet oxygen are limited in much the same way as signals from other two-p
hoton spectroscopic studies (e.g., weak signals that can be masked by scatt
ered radiation). Nevertheless, the two-photon singlet oxygen signals also r
eflect the unique advantages of this nonlinear optical technique (e.g., dep
th penetration in the sample afforded by irradiation in a spectral region v
oid of the more dominant one-photon linear transitions and spatial resoluti
on afforded by irradiation with a focused laser beam).