LiB3O5 (LBO) is one of the most widely used nonlinear optical crystals, therefore the growth of large high quality boules is of major significance to the photonics industry. In the past, LBO single crystals were limited in both size and quality, the latter of which was primarily due to the presence of bubbles, flux inclusions and striations. Furthermore, commercially available material exhibited variable optical absorption. In this research we have perfected the Top-Seeded Solution Growth (TSSG) technique for the growth of LBO single crystals from MoO3-based fluxes. This particular growth process was developed through a thorough study of melt dynamics. Based on the results observed in our modeling experiments, the major growth parameters were optimized. The crystal morphology was modified in order to increase the material yield and eliminate inclusions. As a result we have achieved LBO single crystals of both size and quality, which we believe to be market leading. (C) 2011 Elsevier B.V. All rights reserved.