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1.
J Am Chem Soc ; 146(1): 1053-1061, 2024 Jan 10.
Article En | MEDLINE | ID: mdl-38147824

The use of d-level qudits instead of two-level qubits can largely increase the power of quantum logic for many applications, ranging from quantum simulations to quantum error correction. Magnetic molecules are ideal spin systems to realize these large-dimensional qudits. Indeed, their Hamiltonian can be engineered to an unparalleled extent and can yield a spectrum with many low-energy states. In particular, in the past decade, intense theoretical, experimental, and synthesis efforts have been devoted to develop quantum simulators based on molecular qubits and qudits. However, this remarkable potential is practically unexpressed, because no quantum simulation has ever been experimentally demonstrated with these systems. Here, we show the first prototype quantum simulator based on an ensemble of molecular qudits and a radiofrequency broadband spectrometer. To demonstrate the operativity of the device, we have simulated quantum tunneling of the magnetization and the transverse-field Ising model, representative of two different classes of problems. These results represent an important step toward the actual use of molecular spin qudits in quantum technologies.

2.
Chem Sci ; 12(36): 12046-12055, 2021 Sep 22.
Article En | MEDLINE | ID: mdl-34667570

We show that [VO(TPP)] (vanadyl tetraphenylporphyrinate) is a promising system to implement quantum computation algorithms based on encoding information in multi-level (qudit) units. Indeed, it embeds a nuclear spin 7/2 coupled to an electronic spin 1/2 by hyperfine interaction. This qubit-qudit unit can be exploited to implement quantum error correction and quantum simulation algorithms. Through a combined theoretical and broadband nuclear magnetic resonance study, we demonstrate that the elementary operations of such algorithms can be efficiently implemented on the nuclear spin qudit. Manipulation of the nuclear qudit can be achieved by resonant radio-frequency pulses, thanks to the remarkably long coherence times and the effective quadrupolar coupling induced by the strong hyperfine interaction. This approach may open new perspectives for developing new molecular qubit-qudit systems.

3.
Inorg Chem ; 60(15): 11273-11286, 2021 Aug 02.
Article En | MEDLINE | ID: mdl-34264061

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.

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