The two-photon absorption (TPA), TPA-induced frequency upconversion emission, and two-photon-pumped (TPP) lasing properties of a new dye,trans-4[p-(N-hydroxyethylN-methylamino)stryryl]-N-methylpyridinium iodide (abbreviated as ASPI) were experimentally investigated. This new dye has a moderate TPA cross section (&sgr;2≈3.9×20−20cm4/GW in benzyl alcohol), but exhibits a low lasing threshold and high lasing efficiency when pumped with a 1064 nm pulsed laser beam. Furthermore, the TPA-induced fluorescence yield is strongly dependent on the polarity of the solvent, making it a promising dye for sensing applications. The spectral, temporal, and spatial structures as well as the output/input characteristics of the TPP cavity lasing and the superradiant (cavityless) lasing are systematically measured using a 1 cm path quartz cuvette filled with the ASPI solution or a doped polymer rod. The net conversion efficiency from the absorbed 1064 nm pump pulse energy to the ∼615 nm upconverted cavity lasing energy was found to be as high as ∼17&percent;. ©1997 American Institute of Physics.