Scaling magnets down to where quantum size effects become prominent triggers quantum tunneling of magnetization (QTM), profoundly influencing magnetization dynamics. Measuring magnetization switching in an Fe atomic chain under a carefully tuned transverse magnetic field, we observe a nonmonotonic variation of magnetization lifetimes around a level crossing, known as the diabolic point (DP). Near DPs, local environment effects causing QTM are efficiently suppressed, enhancing lifetimes by three orders of magnitude. Adjusting interatomic interactions further facilitates multiple DPs. Our Letter provides a deeper understanding of quantum dynamics near DPs and enhances our ability to engineer a quantum magnet.

The orbital angular moment of magnetic atoms adsorbed on surfaces is often quenched as a result of an anisotropic crystal field. Due to spin-orbit coupling, what remains of the orbital moment typically delineates the orientation of the electron spin. These two effects limit the scope of information processing based on these atoms to essentially only one magnetic degree of freedom: the spin. In this work, we gain independent access to both the spin and orbital degrees of freedom of a single atom, inciting and probing excitations of each moment. By coordinating a single Fe atom atop the nitrogen site of the Cu₂N lattice, we realize a single-atom system with a large zero-field splitting—the largest reported for Fe atoms on surfaces—and an unquenched uniaxial orbital moment that closely approaches the free-atom value. We demonstrate a full reversal of the orbital moment through a single-electron tunneling event between the tip and Fe atom, a process that is mediated by a charged virtual state and leaves the spin unchanged. These results, which we corroborate using density functional theory and first-principles multiplet calculations, demonstrate independent control over the spin and orbital degrees of freedom in a single-atom system.