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.