G. Amoretti

Engineering the coupling between molecular spin qubits by coordination chemistry

The ability to assemble weakly interacting subsystems is a prerequisite for implementing quantum information processing and generating controlled entanglement. In recent years, molecular nanomagnets have been proposed as suitable candidates for qubit encoding and manipulation. In particular, antiferromagnetic Cr7Ni rings behave as effective spin-1/2 systems at low temperature and show long decoherence times. Here, we show that these rings can be chemically linked to each other and that the coupling between their spins can be tuned by choosing the linker. We also present calculations that demonstrate how realistic microwave pulse sequences could be used to generate maximally entangled states in such molecules.

Molecular engineering of antiferromagnetic rings for quantum computation.

The substitution of one metal ion in a Cr-based molecular ring with dominant antiferromagnetic couplings allows the engineering of its level structure and ground-state degeneracy. Here we characterize a Cr7Ni molecular ring by means of low-temperature specific-heat and torque-magnetometry measurements, thus determining the microscopic parameters of the corresponding spin Hamiltonian. The energy spectrum and the suppression of the leakage-inducing S mixing render the Cr7Ni molecule a suitable candidate for the qubit implementation, as further substantiated by our quantum-gate simulations.

Single molecule magnets for quantum computation

We present recent achievements and perspectives for the encoding of qubits with molecular spin clusters.

Engineering molecular rings for magnetocaloric effect

By substituting one Cr3+(s=3/2) with Cd2+(s=0) in molecular octanuclear rings, a diluted ensemble of identical nanomagnets with a S=3/2 ground state, weakly split in zero field, is obtained. The lattice contribution and the essential parameters of the spin Hamiltonian of these uncompensated antiferromagnetic cyclic spin systems are determined by fitting specific heat data between 0.4 and 20 K in magnetic fields up to 7 T. Different entropy contributions are evaluated and results suggest a possible way of engineering molecular magnets to exploit low temperature magnetocaloric effect.

S-mixing contributions to the high-order anisotropy terms in the effective spin Hamiltonian for magnetic clusters

The magnetic clusters are usually described by an effective Hamiltonian acting in a fixed S space. This single-spin description neglects the mixing between states with different total spin S produced by anisotropic interactions, such as the local crystal field and the magnetic dipole-dipole coupling. We have developed a general and simple procedure, based on a perturbational approach, where the S-mixing effects are included in some new terms to be added to the original effective Hamiltonian. These terms contain some new operators, which depend on the anisotropic interactions and on the difference ΔS between the spin of the states involved in the mixing. Interestingly, these operators are very similar (in some specific cases equal) to the well known Stevens operator equivalents. A list of them for ΔS=1 and ΔS=2 and for second-order anisotropic interactions is presented. The method has been applied to study the S-mixing in two iron nanomagnets, Fe4 and Fe8.

Spin dynamics of heterometallic Cr7M wheels (M=Mn, Zn, Ni) probed by inelastic neutron scattering

Inelastic neutron scattering has been applied to the study of the spin dynamics of Cr-based antiferromagnetic octanuclear rings where a finite total spin of the ground state is obtained by substituting one Cr(III) ion (s = 3/2) with Zn (s = 0), Mn (s = 5/2) or Ni (s = 1) di-cations. Energy and intensity measurements for several intra-multiplet and inter-multiplet magnetic excitations allow us to determine the spin wavefunctions of the investigated clusters. Effects due to the mixing of different spin multiplets have been considered. Such effects proved to be important to correctly reproduce the energy and intensity of magnetic excitations in the neutron spectra. On the contrary to what is observed for the parent homonuclear Cr8 ring, the symmetry of the first excited spin states is such that anticrossing conditions with the ground state can be realized in the presence of an external magnetic field. Heterometallic Cr7M wheels are therefore good candidates for macroscopic observations of quantum effects.

Superposition-model analysis of rare-earth doped BaY 2 F 8

The energy level schemes of four rare-earth dopants (Ce 3+ , Nd 3+ , Dy 3+ , and Er 3+ ) in BaY 2 F 8 , as determined by optical absorption spectra, were fitted with a single-ion Hamiltonian and analysed within Newmans Superposition Model for the crystal field. A unified picture for the four dopants was obtained, by assuming a distortion of the F m ligand cage around the RE site; within the framework of the Superposition Model, this distortion is found to have a marked anisotropic behaviour for heavy rare earths, while it turns into an isotropic expansion of the nearest-neighbours polyhedron for light rare earths. It is also inferred that the substituting ion may occupy an off-center position with respect to the original Y 3+ site in the crystal.

S mixing and quantum tunneling of the magnetization in molecular nanomagnets.

The role of S mixing in the quantum tunneling of the magnetization in nanomagnets has been investigated. We show that the effect on the tunneling frequency is huge and that the discrepancy (more than 3 orders of magnitude in the tunneling frequency) between spectroscopic and relaxation measurements in Fe(8) can be resolved if S mixing is taken into account.

Neutron-scattering investigation of the electronic ground state of neptunium dioxide

Neutron spectroscopy has been applied to study the electronic ground state of NpO2 both in the paramagnetic and in the ordered phase, below Tc=25 K. The magnetic inelastic scattering cross section shows a broad peak which is split into two components and is centred at about 55 meV. This inelastic peak is shown to originate from excitations between the Gamma 8(2) and Gamma 8(1) crystal field quartets. Its position is in agreement with the value estimated by scaling the crystal field potential of UO2 to the Np4+ case. Several mechanisms which could be responsible for the observed splitting are discussed. In the energy range below 15 meV the technique of polarization analysis has been used together with an incident polarized neutron beam to unambiguously separate magnetic from vibronic effects. At low temperature, below 25 K the authors see the appearance of an inelastic line (at an energy transfer of 6.4 meV) that indicates a lifting of the degeneracy of the Gamma 8 ground state. This supports the hypothesis that the phase transition involves the quadrupolar ordering of the Np4+ ions by a collective Jahn-Teller distortion of the oxygen sublattice. The observed amplitude of the splitting is consistent with an oxygen displacement of the order of 0.02 AA, which is below the present limits of resolution of neutron diffraction experiments.

Molecular nanomagnets with switchable coupling for quantum simulation

Molecular nanomagnets are attractive candidate qubits because of their wide inter- and intra-molecular tunability. Uniform magnetic pulses could be exploited to implement one- and two-qubit gates in presence of a properly engineered pattern of interactions, but the synthesis of suitable and potentially scalable supramolecular complexes has proven a very hard task. Indeed, no quantum algorithms have ever been implemented, not even a proof-of-principle two-qubit gate. Here we show that the magnetic couplings in two supramolecular {Cr7Ni}-Ni-{Cr7Ni} assemblies can be chemically engineered to fit the above requisites for conditional gates with no need of local control. Microscopic parameters are determined by a recently developed many-body ab-initio approach and used to simulate quantum gates. We find that these systems are optimal for proof-of-principle two-qubit experiments and can be exploited as building blocks of scalable architectures for quantum simulation.