No Arabic abstract
The physical characterisation and understanding of molecular magnetic materials is one of the most important steps towards the integration of such systems in hybrid spintronic devices. Amongst the many characterisation techniques employed in such a task, Inelastic Neutron Scattering (INS) stands as one of the most powerful and sensitive tools to investigate their spin dynamics. Herein, the magnetic properties and spin dynamics of two dinuclear complexes, namely [(M(hfacac)$_2$)$_2$(bpym)] (where M = Ni$^{2+}$, Co$^{2+}$, abbreviated in the following as Ni$_2$, Co$_2$) are reported. These are model systems that could constitute fundamental units of future spintronic devices. By exploiting the highly sensitive IN5 Cold INS spectrometer, we are able to gain a deep insight into the spin dynamics of Ni$_2$ and to fully obtain the microscopic spin Hamiltonian parameters; while for Co$_2$, a multitude of INS transitions are observed demonstrating the complexity of the magnetic properties of octahedral cobalt-based systems.
The fundamental magnetic interactions of Pr$_{2}$Fe$_{17}$ are studied by inelastic neutron scattering and anisotropy field measurements. Data analysis confirms the presence of three magnetically inequivalent sites, and reveals an exceptionally large value of the exchange field. The unexpected importance of $J$-mixing effects in the description of the ground-state properties of Pr$_{2}$Fe$_{17}$ is evidenced, and possible applications of related compounds are envisaged.
We use polarized inelastic neutron scattering (INS) to study spin excitations of optimally hole-doped superconductor Ba$_{0.67}$K$_{0.33}$Fe$_2$As$_{2}$ ($T_c=38$ K). In the normal state, the imaginary part of the dynamic susceptibility, $chi^{primeprime}(Q,omega)$, shows magnetic anisotropy for energies below $sim$7 meV with c-axis polarized spin excitations larger than that of the in-plane component. Upon entering into the superconducting state, previous unpolarized INS experiments have shown that spin gaps at $sim$5 and 0.75 meV open at wave vectors $Q=(0.5,0.5,0)$ and $(0.5,0.5,1)$, respectively, with a broad neutron spin resonance at $E_r=15$ meV. Our neutron polarization analysis reveals that the large difference in spin gaps is purely due to different spin gaps in the c-axis and in-plane polarized spin excitations, resulting resonance with different energy widths for the c-axis and in-plane spin excitations. The observation of spin anisotropy in both opitmally electron and hole-doped BaFe$_2$As$_2$ is due to their proximity to the AF ordered BaFe$_2$As$_2$ where spin anisotropy exists below $T_N$.
We have studied the frustrated system YBaCo4O7 generally described as an alternating stacking of Kagome and triangular layers of magnetic ions on a trigonal lattice, by single crystal neutron diffraction experiments above the Neel ordering transition. Experimental data reveals pronounced magnetic diffuse scattering, which is successfully modeled by direct Monte-Carlo simulations. Long-range magnetic correlations are found along the c-axis, due to the presence of corner-sharing bipyramids, creating quasi one-dimensional order at finite temperature. In contrast, in the Kagome layers ab-plane, the spin-spin correlation function -displaying a short-range 120 degrees configuration- decays rapidly as typically found in spin-liquids. YBaCo4O7 experimentally realizes a new class of two-dimensional frustrated systems where the strong out-of-plane coupling does not lift the in-plane degeneracy, but instead act as an external field.
The magnetic anisotropy and exchange coupling between spins localized at the positions of 3d transition metal atoms forming two-dimensional metal-organic coordination networks (MOCNs) grown on the Au(111) metal surface are studied. In particular, we consider MOCNs made of Ni or Mn metal centers linked by TCNQ (7,7,8,8-tetracyanoquinodimethane) organic ligands, which form rectangular networks with 1:1 stoichiometry. Based on the analysis of X-ray magnetic circular dichroism (XMCD) data taken at T= 2.5 K, we find that Ni atoms in the Ni-TCNQ MOCNs are coupled ferromagnetically and do not show any significant magnetic anisotropy, while Mn atoms in the Mn-TCNQ MOCNs are coupled antiferromagnetically and do show a weak magnetic anisotropy with in-planemagnetization. We explain these observations using both amodelHamiltonian based on mean-fieldWeiss theory and density functional theory calculations that include spin-orbit coupling. Our main conclusion is that the antiferromagnetic coupling between Mn spins and the in-plane magnetization of the Mn spins can be explained neglecting effects due to the presence of the Au(111) surface, while for Ni-TCNQ the metal surface plays a role in determining the absence of magnetic anisotropy in the system.
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.