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Cooperative quantum cutting mechanism in a spectral converter of Tm3+/Yb3+-codoped tellurite glass is investigated by setting up and solving the theoretical model of rate equations and power propagation equations in MATLAB. Based on the optimal rare-earth (RE) ion concentration and the thickness of the spectral converter, a 155% total power conversion efficiency and a 171% total quantum conversion efficiency have been obtained. For a single-crystalline silicon solar cell, a 20.09% energy conversion efficiency under the optimized solar irradiation compared with a 17.94% energy conversion efficiency under the normalized solar irradiation has been obtained using PC1D, and the simulated relative energy conversion efficiency for the single-crystalline silicon solar cell approaches up to 1.12. These results show that the use of a spectral converter yields better single-crystalline silicon solar-cell performance compared with the normalized solar irradiation. Our results and techniques also provide a framework for investigating and optimizing the Tm3+/Yb3+ couple and other RE-doped spectral converters, potentially enabling a single-crystalline silicon solar cell with an efficiency enhancement.