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Register a new userProbing high-energy electronic excitations using inelastic neutron scattering
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High-energy, local multiplet excitations of the d-electrons are revealed in our inelastic neutron scattering measurements on the prototype magnetic insulator NiO. These become allowed by the presence of both non-zero crystal field and spin-orbit coupling. The observed excitations are consistent with optical, x-ray, and EELS measurements of d-d excitations. This experiment serves as a proof of principle that high-energy neutron spectroscopy is a reliable and useful technique for probing electronic excitations in systems with significant crystal field and spin-orbit interactions.
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Investigating electronic structure and excitations under extreme conditions gives access to a rich variety of phenomena. High pressure typically induces behavior such as magnetic collapse and the insulator-metal transition in 3d transition metals compounds, valence fluctuations or Kondo-like characteristics in $f$-electron systems, and coordination and bonding changes in molecular solids and glasses. This article reviews research concerning electronic excitations in materials under extreme conditions using inelastic x-ray scattering (IXS). IXS is a spectroscopic probe of choice for this study because of its chemical and orbital selectivity and the richness of information it provides. Being an all-photon technique, IXS has a penetration depth compatible with high pressure requirements. Electronic transitions under pressure in 3d transition metals compounds and $f$-electron systems, most of them strongly correlated, are reviewed. Implications for geophysics are mentioned. Since the incident X-ray energy can easily be tuned to absorption edges, resonant IXS, often employed, is discussed at length. Finally studies involving local structure changes and electronic transitions under pressure in materials containing light elements are briefly reviewed.
Polarized neutron inelastic scattering has been used to measure spin excitations in ferromagnetic La$_{0.82}$Sr$_{0.18}$CoO$_{3}$. The magnon spectrum of these spin excitations is well defined at low energies but becomes heavily damped at higher energies, and can be modeled using a quadratic dispersion. We determined a spin wave stiffness constant of $D=94pm 3$,meV,AA$^{2}$. Assuming a nearest-neighbor Heisenberg model we find reasonable agreement between the exchange determined from D and the bulk Curie temperature. Several possible mechanisms to account for the observed spin-wave damping are discussed.
We present data on the magnetic and magneto-elastic coupling in the hexagonal multiferroic manganite LuMnO3 from inelastic neutron scattering, magnetization and thermal expansion measurements. We measured the magnon dispersion along the main symmetry directions and used this data to determine the principal exchange parameters from a spin-wave model. An analysis of the magnetic anisotropy in terms of the crystal field acting on the Mn is presented. We compare the results for LuMnO3 with data on other hexagonal RMnO3 compounds.
We report inelastic neutron scattering measurements of the magnetic excitations in SrFe2As2, the parent of a family of iron-based superconductors. The data extend throughout the Brillouin zone and up to energies of ~260meV. An analysis with the local-moment J_1-J2 model implies very different in-plane nearest-neighbor exchange parameters along the $a$ and $b$ directions, both in the orthorhombic and tetragonal phases. However, the spectrum calculated from the J1-J2 model deviates significantly from our data. We show that the qualitative features that cannot be described by the J1-J2 model are readily explained by calculations from a 5-band itinerant mean-field model.
The study of elementary bosonic excitations is essential toward a complete description of quantum electronic solids. In this context, resonant inelastic X-ray scattering (RIXS) has recently risen to becoming a versatile probe of electronic excitations in strongly correlated electron systems. The nature of the radiation-matter interaction endows RIXS with the ability to resolve the charge, spin and orbital nature of individual excitations. However, this capability has been only marginally explored to date. Here, we demonstrate a systematic method for the extraction of the character of excitations as imprinted in the azimuthal dependence of the RIXS signal. Using this novel approach, we resolve the charge, spin, and orbital nature of elastic scattering, (para-)magnon/bimagnon modes, and higher energy dd excitations in magnetically-ordered and superconducting copper-oxide perovskites (Nd2CuO4 and YBa2Cu3O6.75). Our method derives from a direct application of scattering theory, enabling us to deconstruct the complex scattering tensor as a function of energy loss. In particular, we use the characteristic tensorial nature of each excitation to precisely and reliably disentangle the charge and spin contributions to the low energy RIXS spectrum. This procedure enables to separately track the evolution of spin and charge spectral distributions in cuprates with doping. Our results demonstrate a new capability that can be integrated into the RIXS toolset, and that promises to be widely applicable to materials with intertwined spin, orbital, and charge excitations.
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