We use a combination of microwave fields and free precession to drive the spin of a nitrogen-vacancy (NV) center in diamond on different trajectories on the Bloch sphere and investigate the physical significance of the frame-dependent decomposition of the total phase into geometric and dynamic parts. The experiments are performed on a two-level subspace of the spin-1 ground state of the NV, where the Aharonov-Anandan geometric phase manifests itself as a global phase, and we use the third level of the NV ground-state triplet to detect it. We show that while the geometric Aharonov-Anandan phase retains its connection to the solid angle swept out by the evolving spin, it is generally accompanied by a dynamic phase that suppresses the geometric dependence of the system dynamics. These results offer insights into the physical significance of frame-dependent geometric phases.

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The interaction between a central qubit spin and a surrounding bath of spins is critical to spin-based solid-state quantum sensing and quantum information processing. Spin-bath interactions are typically strongly anisotropic, and rapid physical rotation has long been used in solid-state nuclear magnetic resonance to simulate motional averaging of anisotropic interactions, such as dipolar coupling between nuclear spins. Here, we show that the interaction between electron spins of nitrogen-vacancy centers and a bath of 13 C nuclear spins in a diamond rotated at up to 300 000 rpm introduces decoherence into the system via frequency modulation of the nuclear spin Larmor precession. The presence of an off-axis magnetic field necessary for averaging of the dipolar coupling leads to a rotational dependence of the electron-nuclear hyperfine interaction, which cannot be averaged out with experimentally achievable rotation speeds. Our findings offer new insights into the use of physical rotation for quantum control with implications for quantum systems having motional and rotational degrees of freedom that are not fixed.

Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically-active electron, nuclear spins can be rapidly polarized, controlled and read via lasers and radiofrequency fields. Possessing coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. Unlocking this potential is hampered by precise and inflexible constraints on magnetic field strength and alignment in order to optically induce nuclear polarization, which restricts the scope for further study and applications. In this work, we demonstrate optical nuclear spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at 1 kHz, faster than the nuclear spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in hitherto inaccessible regimes, such as in the presence of a large, time-varying magnetic field that makes an angle of more than 100 • to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation, and even for up to six rotation periods. We combine continuous dynamical decoupling with quantum feedforward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.