Dynamical reorientation of spin multipoles in silicon carbide by transverse magnetic fields

The long-lived and optically addressable high-spin state of the negatively charged silicon vacancy (${V}_{\mathrm{Si}}$) in silicon carbide makes it a promising system for applications in quantum technologies. Most studies of its spin dynamics have been performed under external magnetic fields applied along the symmetry axis. Here, we find that the application of weak magnetic fields perpendicular to the symmetry axis leads to nontrivial behavior caused by the dynamical reorientation of the ${V}_{\mathrm{Si}}$ spin multipole under optical excitation. Particularly, we observe the inversion of the quadrupole-spin polarization in the excited state and the appearance of a dipole-spin polarization in the ground state. The latter is much higher than the thermal polarization and cannot be induced solely by optical excitation. Our theoretical calculations reproduce well all sharp features in the spin-resonance spectra and shine light on the complex dynamics of spin multipoles in these kinds of solid-state systems.