A glass-forming domain is found and studied within the Tl2O-TiO2-TeO2 system. Linear and non-linear optical, thermal and mechanical characteristics were measured and/or theoretically estimated for relevant glasses, and found to be very promising for applications in non-linear optical designs. The chemical, lattice-dynamical and structural effects of the Tl2O and TiO2 modifiers are discussed by using the Raman spectroscopy data. It was concluded that the former modifier favours the non-linear optical properties of the glasses, whereas the latter improves their thermal and mechanical stabilities. (C) 2008 Elsevier Ltd. All rights reserved.