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Register a new userOptical spectroscopy and the nature of the insulating state of rare-earth nickelates
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Using a combination of spectroscopic ellipsometry and DC transport measurements, we determine the temperature dependence of the optical conductivity of NdNiO$_3$ and SmNiO$_{3}$ films. The optical spectra show the appearance of a characteristic two-peak structure in the near-infrared when the material passes from the metal to the insulator phase. Dynamical mean-field theory calculations confirm this two-peak structure, and allow to identify these spectral changes and the associated changes in the electronic structure. We demonstrate that the insulating phase in these compounds and the associated characteristic two-peak structure are due to the combined effect of bond-disproportionation and Mott physics associated with half of the disproportionated sites. We also provide insights into the structure of excited states above the gap.
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We study the temperature dependence of the optical conductivity of rare-earth nickelate films of varying composition and strain close to the antiferromagnetic ordering temperature, TN. Two prominent peaks at 0.6 and 1.3 eV, which are characteristic of the insulating phase, display a small but significant increase in intensity when the material passes from para- to antiferromagnetic. This observation indicates the presence of a positive feedback between antiferromagnetic (AF) and bond disproportionation (BD) order. By analyzing the temperature dependence near TN, and using a Landau-type free-energy expression for BD and AF order, we infer that BD order is a necessary condition for the AF phase to appear, and that the antiferromagnetism contributes to stabilization of the bond disproportionation. This model also explains why hysteresis is particularly strong when the transition into the insulating state occurs simultaneously with antiferromagnetic order.
Based on the electronic band structure obtained from first principles DFT calculations, the opticalspectra of yttrium and neodymium nickelates are computed. We show that the results are in fairagreement with available experimental data. We clarify the electronic transitions at the origin of thefirst two peaks, highlighting the important role of transitions from t2g states neglected in previousmodels. We discuss the evolution of the optical spectra from small to large rare-earth cations andrelate the changes to the electronic band structure.
We report on the synthesis of ultrathin films of highly distorted EuNiO3 (ENO) grown by interrupted pulse laser epitaxy on YAlO3 (YAO) substrates. Through mapping the phase space of nickelate thin film epitaxy, the optimal growth temperatures were found to scale linearly with the Goldschmidt tolerance factor. Considering the gibbs energy of the expanding film, this empirical trend is discussed in terms of epitaxial stabilization and the escalation of the lattice energy due to lattice distortions and decreasing symmetry. These findings are fundamental to other complex oxide perovskites, and provide a route to the synthesis of other perovskite structures in ultrathin-film form.
Rare-earth nickelates exhibit a metal-insulator transition accompanied by a structural distortion that breaks the symmetry between formerly equivalent Ni sites. The quantitative theoretical description of this coupled electronic-structural instability is extremely challenging. Here, we address this issue by simultaneously taking into account both structural and electronic degrees of freedom using a charge self-consistent combination of density functional theory and dynamical mean-field theory, together with screened interaction parameters obtained from the constrained random phase approximation. Our total energy calculations show that the coupling to an electronic instability towards a charge disproportionated insulating state is crucial to stabilize the structural distortion, leading to a clear first order character of the coupled transition. The decreasing octahedral rotations across the series suppress this electronic instability and simultaneously increase the screening of the effective Coulomb interaction, thus weakening the correlation effects responsible for the metal-insulator transition. Our approach allows to obtain accurate values for the structural distortion and thus facilitates a comprehensive understanding, both qualitatively and quantitatively, of the complex interplay between structural properties and electronic correlation effects across the nickelate series.
The metal-insulator transitions and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. Nonetheless, a complete understanding of these materials remains elusive. Here, taking a NdNiO3 thin film as a representative example, we utilize a combination of x-ray absorption and resonant inelastic x-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of the rare-earth nickelates. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for the abundance of oxygen 2p holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that these distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a conventional positive charge-transfer picture, but instead exhibit a negative charge-transfer energy, in line with recent models interpreting the metal to insulator transition in terms of bond disproportionation.
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