Radiofrequency to Microwave Coherent Manipulation of an Organometallic Electronic Spin Qubit Coupled to a Nuclear Qudit

[Image: see text] We report here a comprehensive characterization of a 3d organometallic complex, [V(Cp)(2)Cl(2)] (Cp = cyclopentadienyl), which can be considered as a prototypical multilevel nuclear qudit (nuclear spin I = 7/2) hyperfine coupled to an electronic qubit (electronic spin S = 1/2). By combining complementary magnetic resonant techniques, such as pulsed electron paramagnetic resonance (EPR) and broadband nuclear magnetic resonance (NMR), we extensively characterize its Spin Hamiltonian parameters and its electronic and nuclear spin dynamics. Moreover, we demonstrate the possibility to manipulate the qubit–qudit multilevel structure by resonant microwave and radiofrequency pulses, driving coherent Rabi oscillations between targeted electronuclear states. The obtained results demonstrate that this simple complex is a promising candidate for quantum computing applications.