Accurate Hyperfine Tensors for Solid State Quantum Applications: Case of the NV Center in Diamond

The decoherence of point defect qubits is often governed by the electron spin-nuclear spin hyperfine interaction that can be parameterized by using ab inito calculations in principle. So far most of the theoretical works have focused on the hyperfine interaction of the closest nuclear spins, while the accuracy of the predictions for distinct nuclear spins is barely discussed. We demonstrate for the case of the NV center in diamond that the absolute relative error of the computed hyperfine parameters can exceed 100\% in VASP for weakly coupled nuclear spins. To overcome this issue, we implement an alternative method and report on significantly improved hyperfine values with $O$(1\%) relative mean error at all distances. The provided accurate hyperfine data for the NV center enables high-precision simulation of NV quantum nodes for quantum information processing and positioning of nuclear spins by comparing experimental and theoretical hyperfine data.