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Register a new userSpin dynamics of molecular nanomagnets fully unraveled by four-dimensional inelastic neutron scattering
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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.
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Molecular Nanomagnets have attracted the attention of the scientific community since the rich physics behind their magnetic behaviour make them ideal test-beds for fundamental concepts in quantum mechanics. Sophisticated experiments and targeted research activities have also unveiled their potential for several technological applications. Inelastic neutron scattering is a powerful and widely used technique to investigate the properties of these systems. The new generation of spectrometers, equipped with arrays of position-sensitive detectors, enable to efficiently measure the neutron cross-sections as a function of energy and of the three component of the momentum transfer vector Q, in vast portions of the reciprocal space. Exploiting these capabilities together with the availability of sufficiently large single-crystal samples of MNMs, it is now possible to obtain an unprecedented insight into the coherent spin dynamics of these molecular clusters. This is witnessed by several recent results, that we present in this review. By using the benchmark system Cr$_8$, it has been demonstrated that the richness of the four-dimensional inelastic neutrons scattering technique enables to extract dynamical correlation functions directly from the data. This technique has been also applied to the archetypical single-molecule magnet Mn$_{12}$ to unambiguously characterise its Spin Hamiltonian as well as to portray the entanglement between molecular qubits in (Cr$_7$Ni)$_2$.
We measured two magnetic modes with finite and discrete energies in an antiferromagnetic ordered phase of a geometrically frustrated magnet MgCr2O4 by single-crystal inelastic neutron scattering, and clarified the spatial spin correlations of the two levels: one is an antiferromagnetic hexamer and the other is an antiferromagnetic heptamer. Since these correlation types are emblematic of quasielastic scattering with geometric frustration, our results indicate instantaneous suppression of lattice distortion in an ordered phase by spin-lattice coupling, probably also supported by orbital and charge. The common features in the two levels, intermolecular independence and discreteness of energy, suggest that the spin molecules are interpreted as quasiparticles (elementary excitations with energy quantum) of highly frustrated spins, in analogy with the Fermi liquid approximation.
We present a study of the effects of inelastic scattering on the transport properties of various nanoscale devices, namely H$_2$ molecules sandwiched between Pt contacts, and a spin-valve made by an organic molecule attached to model half-metal ferromagnetic current/voltage probes. In both cases we use a tight-binding Su-Schrieffer-Heeger Hamiltonian and the inelastic effects are treated with a multi-channel method, including Pauli exclusion principle. In the case of the H$_2$ molecule, we find that inelastic backscattering is responsible for the drop of the differential conductance at biases larger than the excitation energy of the lower of the molecular phonon modes. In the case of the spin-valve, we investigate the different spin-currents and the magnetoresistance as a function of the position of the Fermi level with respect to the spin-polarized band edges. In general inelastic scattering reduces the spin-polarization of the current and consequently the magnetoresistance.
Magnetic molecules, modelled as finite-size spin systems, are test-beds for quantum phenomena and could constitute key elements in future spintronics devices, long-lasting nanoscale memories or noise-resilient quantum computing platforms. Inelastic neutron scattering is the technique of choice to probe them, characterizing molecular eigenstates on atomic scales. However, although large magnetic molecules can be controllably synthesized, simulating their dynamics and interpreting spectroscopic measurements is challenging because of the exponential scaling of the required resources on a classical computer. Here, we show that quantum computers have the potential to efficiently extract dynamical correlations and the associated magnetic neutron cross-section by simulating prototypical spin systems on a quantum hardware. We identify the main gate errors and show the potential scalability of our approach. The synergy between developments in neutron scattering and quantum processors will help design spin clusters for future applications.
The magnetization of the prototypical molecular magnet Mn12-acetate exhibits a series of sharp steps at low temperatures due to quantum tunneling at specific resonant values of magnetic field applied along the easy c-axis. An abrupt reversal of the magnetic moment of such a crystal can also occur as an avalanche, where the spin reversal proceeds along a deflagration front that travels through the sample at subsonic speed. In this article we review experimental results that have been obtained for the ignition temperature and the speed of propagation of magnetic avalanches in molecular nanomagnets. Fits of the data with the theory of magnetic deflagration yield overall qualitative agreement. However, numerical discrepancies indicate that our understanding of these avalanches is incomplete.
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