Two coumarin derived dyes (compounds La and L) have been synthesized in high yields by Schiff base condensation. On probing with a femtosecond laser, none of these compounds show any two-photon activity in the wavelength range, 760-860 nm. However, La in presence of Zn(II) and L in presence of Mg(II), exhibit large two-photon absorption as well as emission in the same wavelength range. Theoretical calculations at the B3LYP functional with 6-31G and LanL2DZ mixed basis set under DFT formalism support experimental results. © 2010 Elsevier B.V. All rights reserved.