We report the results of inelastic neutron scattering experiments performed with triple-axis spectrometers to investigate the low-temperature collective dynamics in the ordered phase of uranium dioxide. The results are in excellent agreement with the predictions of mean-field RPA calculations emphasizing the importance of multipolar superexchange interactions. By comparing neutron scattering intensities in different polarization channels and at equivalent points in different Brillouin zones, we show the mixed magneto-vibrational-quadrupolar character of the observed excitations. The high energy resolution afforded by the cold triple-axis spectrometer allowed us to study in detail the magnon-phonon interaction giving rise to avoided crossings along the $[00xi]$ reciprocal space direction.
Entanglement between individual spins can be detected by using thermodynamics quantities as entanglement witnesses. This applies to collective spins also, provided that their internal degrees of freedom are frozen, as in the limit of weakly-coupled nanomagnets. Here, we extend such approach to the detection of entanglement between subsystems of a spin cluster, beyond such weak-coupling limit. The resulting inequalities are violated in spin clusters with different geometries, thus allowing the detection of zero- and finite-temperature entanglement. Under relevant and experimentally verifiable conditions, all the required expectation values can be traced back to correlation functions of individual spins, that are now made selectively available by four-dimensional inelastic neutron scattering.
We introduce a scheme to perform quantum-information processing that is based on a hybrid spin-photon qubit encoding. The proposed qubits consist of spin-ensembles coherently coupled to microwave photons in coplanar waveguide resonators. The quantum gates are performed solely by shifting the resonance frequencies of the resonators on a ns timescale. An additional cavity containing a Cooper-pair box is exploited as an auxiliary degree of freedom to implement two-qubit gates. The generality of the scheme allows its potential implementation with a wide class of spin systems.
We present a flexible and effective ab-initio scheme to build many-body models for molecular nanomagnets, and to calculate magnetic exchange couplings and zero-field splittings. It is based on using localized Foster-Boys orbitals as one-electron basis. We apply this scheme to three paradigmatic systems, the antiferromagnetic rings Cr8 and Cr7Ni and the single molecule magnet Fe4. In all cases we identify the essential magnetic interactions and find excellent agreement with experiments.
Molecular nanomagnets are among the first examples of spin systems of finite size and have been test-beds for addressing a range of elusive but important phenomena in quantum dynamics. In fact, for short-enough timescales the spin wavefunctions evolve coherently according to the an appropriate cluster spin-Hamiltonian, whose structure can be tailored at the synthetic level to meet specific requirements. Unfortunately, to this point it has been impossible to determine the spin dynamics directly. If the molecule is sufficiently simple, the spin motion can be indirectly assessed by an approximate model Hamiltonian fitted to experimental measurements of various types. Here we show that recently-developed instrumentation yields the four-dimensional inelastic-neutron scattering function S(Q,E) in vast portions of reciprocal space and enables the spin dynamics to be determined with no need of any model Hamiltonian. We exploit the Cr8 antiferromagnetic ring as a benchmark to demonstrate the potential of this new approach. For the first time we extract a model-free picture of the quantum dynamics of a molecular nanomagnet. This allows us, for example, to examine how a quantum fluctuation propagates along the ring and to directly test the degree of validity of the N{e}el-vector-tunneling description of the spin dynamics.
Quantum simulators are controllable systems that can be used to simulate other quantum systems. Here we focus on the dynamics of a chain of molecular qubits with interposed antiferromagnetic dimers. We theoretically show that its dynamics can be controlled by means of uniform magnetic pulses and used to mimic the evolution of other quantum systems, including fermionic ones. We propose two proof-of-principle experiments, based on the simulation of the Ising model in transverse field and of the quantum tunneling of the magnetization in a spin-1 system.
We investigate the magnetic properties of three Mn$_6$ single molecule magnets by means of inelastic neutron scattering and frequency domain magnetic resonance spectroscopy. The experimental data reveal that small structural distortions of the molecular geometry produce a significant effect on the energy level diagram and therefore on the magnetic properties of the molecule. We show that the giant spin model completely fails to describe the spin level structure of the ground spin multiplets. We analyze theoretically the spin Hamiltonian for the low spin Mn$_6$ molecule (S=4) and we show that the excited $S$ multiplets play a key role in determining the effective energy barrier for the magnetization reversal, in analogy to what was previously found for the two high spin Mn6 (S=12) molecules [S. Carretta et al., Phys. Rev. Lett. 100, 157203 (2008)].
We study the magnetization and the spin dynamics of the Cr$_7$Ni ring-shaped magnetic cluster. Measurements of the magnetization at high pulsed fields and low temperature are compared to calculations and show that the spin Hamiltonian approach provides a good description of Cr$_7$Ni magnetic molecule. In addition, the phonon-induced relaxation dynamics of molecular observables has been investigated. By assuming the spin-phonon coupling to take place through the modulation of the local crystal fields, it is possible to evaluate the decay of fluctuations of two generic molecular observables. The nuclear spin-lattice relaxation rate $1/T_1$ directly probes such fluctuations, and allows to determine the magnetoelastic coupling strength.
Inelastic neutron scattering has been used to determine the microscopic Hamiltonian describing two high-spin variants of the high-anisotropy Mn$_6$ nanomagnet. The energy spectrum of both systems is characterized by the presence of several excited total-spin multiplets partially overlapping the S=12 ground multiplet. This implies that the relaxation processes of these molecules are different from those occurring in prototype giant-spin nanomagnets. In particular, we show that both the height of the energy barrier and resonant tunnelling processes are greatly influenced by low-lying excited total-spin multiplets.
