The two-photon absorption (TPA) properties of a novel group of pyrylium-based compounds were studied. The molecules of this group were synthesized by systematically changing the chemical structure of a specific substituent in an initial chromophore. TPA cross-sections as large as 1.8 x 10(-47) cm(4) s photon(-1) and high quantum yields were obtained. The results combined with the low cost and ease of synthesis of these compounds make them candidates for TPA applications. Particularly, three-dimensional data storage in polymer matrices of the synthesized compounds was realized through the photobleaching process. The high efficiency of recording and the submicron resolution reveal the great potential of this group of molecules as memory materials. (C) 2003 Elsevier Science B.V. All rights reserved.