Abstract
We report here a comprehensive characterization of a 3d organometallic complex, [V(Cp)2Cl2] (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.
Highlights
In the past few years, the research on S = 1/2 molecular spin systems, which can be used as the building blocks of a potential quantum computer, experienced a surge of interest.[1−3] Such elementary units are two-level quantum systems called qubits
A distinctive feature of molecular spin systems, compared to other consolidated platforms for quantum computing (QC),[18−27] is the ease of obtaining single-quantum objects featuring more than two levels: such systems, with a number of degrees of freedom d > 2, are known as qudits.[28−35] Their multilevel structure can be characterized in detail by exploiting different experimental and theoretical techniques,[36−38] and states encoded in such levels can be manipulated by electromagnetic pulses in the microwave[39−43] or radiofrequency ranges.[44]
The molecular structure of 1 is that of a bent-metallocene complex with the central metal ion coordinated by two cyclopentadienyl ligands (Cp) and two additional coordinating ligands, here chloride
Summary
The single-crystal EPR study provided a sound set of electronic spin Hamiltonian parameters and solved the issue related to the orientation of the anisotropy axes in this molecule.[67,73] refs 67 and 73 reported remarkable differences in the orientation of the anisotropy axes with respect to the molecular structure despite the similarity of the investigated complexes. This has to be attributed to the absence of a reliable structure determination for 1 and 2 at the time of ref 67. Spectral separation of the different hyperfine lines (needed to separately detect different dephasing errors) is clearly shown in the EPR spectra of Figure 2 and S5
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