We propose high-fidelity controlled-NOT (CNOT) gates in a hybrid system of polar molecules and Rydberg atoms based on the unconventional Rydberg pumping mechanism. By combining the rich internal structure of polar molecules with the strong dipole-dipole interactions of Rydberg atoms, we realize both two-to-one and one-to-two gate configurations. Numerical simulations show that the gate performance is robust against spontaneous emission from Rydberg states. The approach naturally extends to larger systems, as demonstrated by four-qubit implementations achieving three-to-one and one-to-three CNOT gates with fidelities exceeding 99%. These results highlight hybrid molecule-Rydberg atom architectures as a promising platform for scalable quantum information processing.

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