Different Termination Diamond Yb Vacancy Color Centers on the (110) Surface: <i>Ab Initio</i> and Machine-Learning Molecular Dynamics

Yb vacancy color centers on diamond (110) surfaces are promising candidates for long-coherence solid-state qubits and scalable quantum networks. However, their performance is strongly affected by surface termination, where the mechanism of charge redistribution and its impact on defect dynamics remain unclear. Here, we combine first-principles calculations and machine-learning molecular dynamics (MLMD) to systematically study F-, H-, N-, and O-terminated surfaces. The results reveal that the electronegativity of the terminating atom governs interfacial charge rearrangement, which, in turn, dictates the key quantum properties of Yb centers. The highly electronegative F termination induces the strongest surface dipole and the most significant charge transfer from the lattice, resulting in superior electronic and structural stability. Electron localization and COHP analyses show that strong C-F bonds effectively passivate dangling bonds and eliminate near-Fermi defect states. Furthermore, F termination suppresses electron-phonon coupling-induced decoherence and exhibits minimal atomic fluctuation in MLMD simulations. This synergy between electronic and dynamic stability identifies F termination as the most favorable configuration for engineering robust, high-performance Yb color centers in diamond.