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The effect of alkali fluoride on the photoluminescence properties of Tb3+ doped on the phosphate glass was discovered. However, the composition of the glass samples were 20Li2O–10AlF3–69P2O5–1Tb2O3 (LAPTb) and 20Li2O–10AlF3–10NaF–59P2O5–1Tb2O3 (LANPTb). To study optical properties were examined through their absorption and luminescence spectra. Luminescence spectra were investigated by photoluminescence. Characteristic luminescence bands corresponding to electronic transitions of terbium ions (Tb3+) were detected under two direct excitations of Tb3+ ions. Upon 377 nm excitation, the glass samples were obtained transition terbium 5D4 → 7F5 at 544 nm showed a green laser. The decay time Tb3+ for the 5D4 level has been confirmed and the result was 2.865 ms and 2.982 ms corresponding to LAPTb was LANPTb, respectively. The green laser application has been investigated by a CIE-color-coordinates diagram with a color purity is ~73%.