Lithium containing chalcogenide single crystals have become very promising materials for photonics and radiation detection. Detection applications include nuclear nonproliferation, neutron science, and stellar investigations for the search of life. Synthesis and single crystal growth methods for lithium containing chalcogenide, specifically LiIn1-xGaxSe2, single crystals are discussed. This study elucidates the possibility of improving neutron detection by reducing the indium capture contribution; with the incorporation of the lithium-6 isotope, gallium substitution may overcome the neutron detection efficiency limitation of 6LiInSe2 due to appreciable neutron capture by the indium-115 isotope. As a figure of merit, the ternary parent compounds (6)LiInSe2 and 6LiGaSe2 were included in this study. Quality crystals can be obtained utilizing the vertical Bridgman method to produce quaternary compounds with tunable optical properties. Quaternary crystals of varying quality depending on the gallium concentration, approximately 5x5x2 mm3 or larger in volume, were harvested, analyzed and revealed tunable absorption characteristics between 2.8-3.4 eV.