1：Experimental Design and Method Selection:

Single crystals of Nd3+:CaNb2O6 and Nd3+:La3+:CaNb2O6 were grown by the Czochralski method. Atomistic computer simulation of RE3+ (RE3+=Nd3+, La3+) ions incorporation in the CaNb2O6 crystal based on energy minimization with a Born-like description of lattice has been performed using the General Utility Lattice Program (GULP).

2：Sample Selection and Data Sources:

The raw materials of 1 at.% Nd3+:CaNb2O6 and 1 at.% Nd3+: 1 at.% La3+:CaNb2O6 were synthesized by the solid-state reaction method.

3：List of Experimental Equipment and Materials:

Chemicals used were CaCO3, Nb2O5, Nd2O3 and La2O3 with same purity of 99.99%. The crystals were grown along its c-axis in an iridium crucible in a nitrogen atmosphere containing 1% oxygen.

4：99%. The crystals were grown along its c-axis in an iridium crucible in a nitrogen atmosphere containing 1% oxygen. Experimental Procedures and Operational Workflow:

4. Experimental Procedures and Operational Workflow: The pulling rate was 1-2 mm/h and the rotating rate was 5-15 rpm during growth. After growth, the crystal was cooled down to room temperature at a speed of 20-40oC/h. The as-grown single crystals were annealed in an annealing furnace in air to eliminate the oxygen defects and the stress formed during growth.

5：Data Analysis Methods:

The fluorescence properties of the Nd3+:CaNb2O6 and Nd3+:La3+:CaNb2O6 have been studied. Efficient fundamental and self-SRS lasers have been achieved in the Nd3+:La3+:CaNb2O6.