A convenient method for synthesizing alpha-(1,2,4-triazolo[1,5-a]pyrimidine-2-sulfonyl)methane derivatives, 3 and 4, by the well known Knoevenagel reaction, in one step, is described. The two chromophores are stilbene-type chromophores containing the same D-pi-A structures and end-capped with aromatic group as their donors. Measured with femtosecond multipass Ti:sapphire amplifier as irradiation source (pumped by the laser at 800 nm), the two chromophores show efficient two-photon induced orange red fluorescence emission. The experimental results indicate that the numbers of branches of the tw...