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Improving the performance of molecular qubits is a fundamental milestone towards unleashing the power of molecular magnetism in the second quantum revolution. Taming spin relaxation and decoherence due to vibrations is crucial to reach this milestone, but this is hindered by our lack of understanding on the nature of vibrations and their coupling to spins. Here we propose a synergistic approach to study a prototypical molecular qubit. It combines inelastic X-ray scattering to measure phonon dispersions along the main symmetry directions of the crystal and spin dynamics simulations based on DFT. We show that the canonical Debye picture of lattice dynamics breaks down and that intra-molecular vibrations with very-low energies of 1-2 meV are largely responsible for spin relaxation up to ambient temperature. We identify the origin of these modes, thus providing a rationale for improving spin coherence. The power and flexibility of our approach open new avenues for the investigation of magnetic molecules with the potential of removing roadblocks toward their use in quantum devices.
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We use diffuse and inelastic x-ray scattering to study the formation of an incommensurate charge-density-wave (I-CDW) in BaNi_{2}As_{2}, a candidate system for charge-driven electronic nematicity. Intense diffuse scattering is observed around the modulation vector of the I-CDW, Q_{I-CDW}. It is already visible at room temperature and collapses into superstructure reflections in the long-range ordered state where a small orthorhombic distortion occurs. A clear dip in the dispersion of a low-energy transverse optical phonon mode is observed around Q_{I-CDW}. The phonon continuously softens upon cooling, ultimately driving the transition to the I-CDW state. The transverse character of the soft-phonon branch elucidates the complex pattern of the I-CDW satellites observed in the current and earlier studies and settles the debated unidirectional nature of the I-CDW. The phonon instability and its reciprocal space position are well captured by our ab initio calculations. These, however, indicate that neither Fermi surface nesting, nor enhanced momentum-dependent electron-phonon coupling can account for the I-CDW formation, demonstrating its unconventional nature.
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A new diffractometer is now available to the general user community at the ESRF. The new diffractometer is a side station of the high-resolution inelastic X-ray scattering spectrometer on beamline ID28 and is located in the same experimental hutch. Both instruments can be operated simultaneously. The new diffractometer combines a fast and low-noise hybrid pixel detector with a variable diffraction geometry. The beam spot on the sample is 50â µm × 50â µm, where focusing is achieved by a combination of Be lenses and a KB mirror. Wavelengths from 0.5 to 0.8â Å can be used for the diffraction experiments. The setup is compatible with a variety of sample environments, allowing studies under non-ambient conditions. The diffractometer is optimized to allow a rapid survey of reciprocal space and diffuse scattering for the identification of regions of interest for subsequent inelastic scattering studies, but can also be employed as a fully independent station for structural studies from both powder and single-crystal diffraction experiments. Several software packages for the transformation and visualization of diffraction data are available. An analysis of data collected with the new diffractometer shows that the ID28 side station is a state-of-the-art instrument for structural investigations using diffraction and diffuse scattering experiments.
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Magneto-electric multiferroics exemplified by TbMnO(3) possess both magnetic and ferroelectric long-range order. The magnetic order is mostly understood, whereas the nature of the ferroelectricity has remained more elusive. Competing models proposed to explain the ferroelectricity are associated respectively with charge transfer and ionic displacements. Exploiting the magneto-electric coupling, we used an electric field to produce a single magnetic domain state, and a magnetic field to induce ionic displacements. Under these conditions, interference between charge and magnetic x-ray scattering arose, encoding the amplitude and phase of the displacements. When combined with a theoretical analysis, our data allow us to resolve the ionic displacements at the femtoscale, and show that such displacements make a substantial contribution to the zero-field ferroelectric moment.
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Nonresonant x-ray magnetic scattering has been used to study the magnetic structure of multiferroic TbMnO3 in its ferroelectric phase. Circularly polarized x rays were combined with full polarization analysis of the scattered beam to reveal important new information on the magnetic structure of this canonical multiferroic. An applied electric field is shown to create essentially a single magnetic domain state in which the cycloidal order on the Mn sublattice rotates either clockwise or anticlockwise depending on the sign of the field. It is demonstrated how this technique provides sensitivity to the absolute sense of rotation of the Mn moments and to components of the ordering on the Tb sublattice and phase shifts that earlier neutron diffraction experiments could not resolve.
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We show that the magnetic state in rather thick Cr films can be finely tuned via hydrogen uptake into adjacent vanadium layers at rather low hydrogen pressures. By changing the hydrogen concentration and, hence, the electronic structure in the V layers, it is possible to affect the global properties of spin-density waves (SDWs) in Cr layers, including the SDW period and the Néel temperature. We provide direct experimental evidence that hydrogen uptake into V layers can be used to switch between incommensurate and commensurate SDW states in a reproducible way.
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We have performed extended x-ray absorption fine-structure (EXAFS) spectroscopy on a 2.8% Cr-doped V(2)O(3) sample, with the aim of studying its structural evolution in a wide temperature range across the paramagnetic-antiferromagnetic insulating phase transition at T(c). The data were registered with two different set-ups in fluorescence and transmission geometries, for polarized and unpolarized spectra, respectively. Our idea, based on previous experiments reported in the literature, is that extended structural modifications of the nominal trigonal symmetry are present in the paramagnetic insulating phase for several tens of degrees above T(c), involving further-nearest-neighbor vanadium ions. Our data confirm that the paramagnetic insulating phase is not structurally homogeneous in a temperature range of about 30 K around T(c), where local distortions of monoclinic symmetry involving further-nearest neighbors are present. Moreover, the analysis of the absorption profile at Cr K-edge suggests that Cr ions enter the lattice randomly. We finally analyze our findings in light of current theoretical models.
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A new experimental station at ESRF beamline ID20 is presented which allows magnetic and resonant X-ray scattering experiments in the energy range 3-25 keV to be performed under extreme conditions. High magnetic field up to 10 T, high pressure up to 30 kbar combined with low temperatures down to 1.5 K are available and experiments can be performed at the M-edges of actinide elements, L-edges of lanthanides and K-edges of transition metals.
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We have measured hard x-ray photoemission spectra of pure vanadium sesquioxide (V(2)O(3)) across its metal-insulator transition. We show that, in the metallic phase, a clear correlation exists between the shakedown satellites observed in the vanadium 2p and 3p core-level spectra and the coherent peak measured at the Fermi level. Comparing experimental results and dynamical mean-field theory calculations, we estimate the Hubbard energy U in V(2)O(3) (4.20+/-0.05 eV). From our bulk-sensitive photoemission spectra we infer the existence of a critical probing depth for investigating electronic properties in strongly correlated solids.
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Coherent x-ray diffraction experiments have been performed on high quality crystals of the charge density wave (CDW) system K0.3MoO3. The satellite reflections associated with the CDW have been measured as a function of the 20-microm-diameter beam position. For some positions, regular fringes have been observed. We show that this observation is consistent with the presence of a single CDW dislocation. Beyond charge density wave systems, this experiment shows that coherent x-ray diffraction is a suitable tool to probe topological defects embedded in the bulk.
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Powder neutron diffraction and resonant x-ray scattering measurements from a single crystal have been performed to study the low-temperature state of the 2D frustrated, quantum-Heisenberg system Li2VOSiO4. Both techniques indicate a collinear antiferromagnetic ground state, with propagation vector k=(1 / 2 1 / 2 0), and magnetic moments in the a-b plane. Contrary to previous reports, the ordered moment at 1.44 K, m=0.63(3)micro(B), is very close to the value expected for the square lattice Heisenberg model ( approximately 0.6micro(B)). The magnetic order is three dimensional, with antiferromagnetic a-b layers stacked ferromagnetically along the c axis. Neither x-ray nor neutron diffraction shows evidence for a structural distortion between 1.6 and 10 K.
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A combination of neutron elastic and inelastic, resonant x-ray scattering, and 57Fe Mössbauer experiments are used to determine the unusual magnetic ground state of CeFe2. The complementarities between different time-scale techniques may allow one to understand the dynamic features of the ground state in CeFe2 and its pseudobinary compounds, and how the frustration of Fe tetrahedra leads the appearance of antiferromagnetic fluctuations in the presence of ferrimagnetism. The resulting model can be used to rationalize many of the unusual and conflicting experimental results reported for this material in the literature.
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A thorough tensor analysis of the Bragg-forbidden reflection (00.3)(h) in corundum systems having a global center of inversion, such as V2O3 and alpha-Fe2O3, shows that anomalous x-ray resonant diffraction can access chiral properties related to the dipole-quadrupole (E1-E2) channel via an interference with the pure quadrupole-quadrupole (E2-E2) process. This is also confirmed by independent ab initio numerical simulations. In such a way, it becomes possible to detect chiral quantities in systems where dichroic absorption techniques are ineffective.
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We present the results of resonant x-ray scattering experiments on KCuF3. Structurally forbidden reflections, corresponding to magnetic and 3d-orbital long-range order, have been observed. Integrated intensities have been measured as a function of incident energy, polarization, azimuthal angle, and temperature. The results give evidence for a strong coupling between orbital and spin degrees of freedom. The interplay between magnetic and orbital order parameters is revealed by the temperature dependence of the intensity of orbital Bragg peaks.
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The first direct observation of charge order of Ni(3+delta(')) and Ni(3-delta) by resonant x-ray scattering experiments in an epitaxial film of NdNiO3 is reported. A quantitative value of delta+delta(') = (0.45 +/- 0.04)e was obtained. The temperature dependence of the charge order deviates significantly from those of the magnetic moment and crystallographic structure. This might be an indication of a difference in their fluctuation time scales. These observations are discussed in terms of the temperature-driven metal-insulator transition in the RNiO3 family.
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Synchrotron experiments with uranium antiferromagnetic compounds have discovered large ( >1000) enhancements of the magnetic scattering intensities at the K edges of nominally nonmagnetic anions, e.g., Ga and As. The width in energy, the position with respect to the white line, and the azimuthal and polarization dependencies permit one to associate the signal with transitions of E1 dipole symmetry from 1s to 4p states. In momentum space, the signal exhibits long-range order at the antiferromagnetic wave vector. We discuss possible channels capable of generating the observed enhancements.
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We report the first observation of a nonreciprocal x-ray linear dichroism caused by the time-reversal odd, real part zeta of the complex gyrotropy tensor zeta(*) which is dominated by electric dipole-electric quadrupole E1E2 interference terms. A nonreciprocal transverse anisotropy was observed in the low temperature insulating phase of a Cr doped V2O3 Mott crystal when a single antiferromagnetic domain was grown by magnetoelectric annealing along the hexagonal c axis. This new element (edge) specific spectroscopy could nicely complement x-ray magnetic circular dichroism which is silent for antiferromagnetic materials.