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Register a new userResolving interfacial charge transfer in titanate superlattices using resonant X-ray reflectometry
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Charge transfer in oxide heterostructures can be tuned to promote emergent interfacial states, and accordingly, has been the subject of intense study in recent years. However, accessing the physics at these interfaces, which are often buried deep below the sample surface, remains difficult. Addressing this challenge requires techniques capable of measuring the local electronic structure with high-resolution depth dependence. Here, we have used linearly-polarized resonant X-ray reflectometry (RXR) as a means to visualize charge transfer in oxide superlattices with atomic layer precision. From our RXR measurements, we extract valence depth profiles of SmTiO$_3$ (SmTO)/SrTiO$_3$ (STO) heterostructures with STO quantum wells varying in thickness from 5 SrO planes down to a single, atomically thin SrO plane. At the polar-nonpolar SmTO/STO interface, an electrostatic discontinuity leads to approximately half an electron per areal unit cell transferred from the interfacial SmO layer into the neighboring STO quantum well. We observe this charge transfer as a suppression of the t$_{2g}$ absorption peaks that minimizes contrast with the neighboring SmTO layers at those energies and leads to a pronounced absence of superlattice peaks in the reflectivity data. Our results demonstrate the sensitivity of RXR to electronic reconstruction at the atomic scale, and establish RXR as a powerful means of characterizing charge transfer at buried oxide interfaces.
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We report a high-resolution resonant inelastic x-ray scattering study of La2CuO4. A number of spectral features are identified that were not clearly visible in earlier lower-resolution data. The momentum dependence of the spectral weight and the dispersion of the lowest energy excitation across the insulating gap have been measured in detail. The temperature dependence of the spectral features was also examined. The observed charge transfer edge shift, along with the low dispersion of the first charge transfer excitation are attributed to the lattice motion being coupled to the electronic system. In addition, we observe a dispersionless feature at 1.8 eV, which is associated with a d-d crystal field excitation.
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.
(LaNiO3)n/(LaMnO3)2 superlattices were grown using ozone-assisted molecular beam epitaxy, where LaNiO3 is a paramagnetic metal and LaMnO3 is an antiferromagnetic insulator. The superlattices exhibit excellent crystallinity and interfacial roughness of less than 1 unit cell. X-ray spectroscopy and dichroism measurements indicate that electrons are transferred from the LaMnO3 to the LaNiO3, inducing magnetism in LaNiO3. Magnetotransport measurements reveal a transition from metallic to insulating behavior as the LaNiO3 layer thickness is reduced from 5 unit cells to 2 unit cells and suggest a modulated magnetic structure within LaNiO3.
Strongly correlated materials are characterized by the presence of electron-electron interactions in their electronic structure. They often have remarkable properties and transitions between competing phases of very different electronic and magnetic order. This thesis focuses on strongly correlated $f$-electron compounds containing Ce, Sm, and U. These materials exhibit a so-called heavy-fermion or Kondo-lattice behavior. They can become insulating due to hybridization effects (Kondo-insulator) or develop multipolar (hidden) order. Kondo insulators have recently been discussed in the context of strongly correlated topological insulators. This new aspect caused an enormous activity in the field of Kondo insulators, theoretically as well as experimentally. Multipolar order as well as the formation of a Kondo insulating state strongly depend on the symmetry of the $f$ states involved. Also the character of the surface states in a topological insulator is determined by the properties of the bulk states. Therefore the scope of this thesis has been to unveil the underlying symmetries of the bulk $f$ states. Here the compounds CeB$_6$, UO$_2$, and URu$_2$Si$_2$, which exhibit multipolar order, as well as the Kondo insulators (semimetals) SmB$_6$ and CeRu$_4$Sn$_6$ have been studied.
We report a resonant inelastic x-ray scattering study of the dispersion relations of charge transfer excitations in insulating La$_2$CuO$_4$. These data reveal two peaks, both of which show two-dimensional characteristics. The lowest energy excitation has a gap energy of $sim 2.2$ eV at the zone center, and a dispersion of $sim 1$ eV. The spectral weight of this mode becomes dramatically smaller around ($pi$, $pi$). The second peak shows a smaller dispersion ($sim 0.5$ eV) with a zone-center energy of $sim 3.9$ eV. We argue that these are both highly dispersive exciton modes damped by the presence of the electron-hole continuum.
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