3D optical data storage can benefit from the non-linear process of two-photon absorption (TPA). If some chromphores with large TPA cross section are introduced into the diarylethene to enhance its two-photon absorptivities, it is expected to be good recording media for 3D optical data storage. The authors have synthesized four diarylperfluorocyclopentene (DPFCP) derivates for the purpose of developing two-photon 3D optical data storage. The nonlinear two-photon absorption (TPA) properties of the compounds were examined, and the reaction and excited state relaxation dynamics after two-photon excitation were investigated. The TPA cross sections of 2-position DPFCPs were measured by means of TPIF (two-photon induced fluorescence) method, and the highest is 48×10-50cm4"s"photo-1"molecule-1. The compounds were successfully applied in two-photon 3D optical data storage based on single beam two-photon femtosecond writing and one-photon fluorescence reading. Ten-layer clear images on DPFCP/PMMA film were obtained, and the data storage density is high to 2.0×1011 bits/cm3.© (2005) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.