Journal of Chemical Theory and Computation • Vol 21 • No 16
Hyperfine Coupling Constants on Quantum Computers: Performance, Errors, and Future Prospects
2025
We present the first implementation and computation of electron spin resonance isotropic hyperfine coupling constants (HFCs) on a quantum hardware. As illustrative test cases, we compute the HFCs for the hydroxyl radical (OH<sup>•</sup>), nitric oxide (NO<sup>•</sup>), and triplet hydroxyl cation (OH<sup>+</sup>). Our approach integrates the qubit-ADAPT method with unrestricted orbital optimization in an active space framework. To accurately measure the necessary spin one-electron-reduced density matrices on curre…