With the use of a cavity-dumped, synchronously pumped dye laser for ex
citation, two-photon fluorescence cross sections are approximately eig
ht orders of magnitude smaller than those for one-photon excitation. T
hus, examination of dilute solutions has been achieved only with great
difficulty. Any successful instrumentation will require that the blan
k be essentially eliminated. To this end, time-filtered detection has
been combined with two-photon excitation and spatial filtering to prod
uce fluorometric detection limits of 38 pM for 9,10-diphenylanthracene
and 8.6 pM for alpha-NPO. It is believed that this latter value is th
e lowest concentration yet reported for two-photon spectroscopy in flu
id solution. The instrumentation and data processing are described. Ad
ditionally, a comparison is made with the performance of other recent
alternative approaches involving spatial filtering and second harmonic
detection.