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Register a new userTunable disorder and localization in the rare-earth nickelates
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The rare-earth nickelates are a rich playground for transport properties, known to host non-Fermi liquid character, resistance saturation and metal-insulator transitions. We report a study of transport in LaNiO3 in the presence of tunable disorder induced by irradiation. While pristine LaNiO3 samples are metallic, highly irradiated samples show insulating behaviour at all temperatures. Using irradiation fluence as a tuning handle, we uncover an intermediate region hosting a metal-insulator transition. This transition falls within the Mott-Ioffe-Regel regime wherein the mean free path is comparable to lattice spacing. In the high temperature metallic regime, we find a transition from non-Fermi liquid to a Fermi-liquid-like character. On the insulating side of the metal-insulator transition, we find behaviour that is consistent with weak localization. This is reflected in magnetoresistance that scales with the square of the field and in resistivity. In the highly irradiated insulating samples, we find good agreement with variable range hopping, consistent with Anderson localization. We find qualitatively similar behaviour in thick PrNiO3 films as well. Our results demonstrate that ion irradiation can be used to tailor transport, serving as an excellent tool to study the physics of localization.
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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.
The properties of AMO3 perovskite oxides, where M is a 3d transition metal, depend strongly on the level of covalency between the metal d and oxygen p orbitals. With their complex spin orders and metal-insulator transition, rare-earth nickelates verge between dominantly ionic and covalent characters. Accordingly, the nature of their ground state is highly debated. Here, we reconcile the ionic and covalent visions of the insulating state of nickelates. Through first-principles calculations, we show that it is reminiscent of the ionic charge disproportionation picture (with strictly low-spin 4+ and high-spin 2+ Ni sites) while exhibiting strong covalence effects with oxygen electrons shifted toward the depleted Ni cations, mimicking a configuration with identical Ni sites. Our results further hint at strategies to control electronic and magnetic phases of transition metal oxide perovskites.
We present a systematic density functional theory (DFT) plus Hubbard $U$ study of structural trends and the stability of different magnetically ordered states across the rare-earth nickelate series, $R$NiO$_3$, with $R$ from Lu to La. In particular, we investigate how the magnetic order, the change of the rare-earth ion, and the Hubbard interaction $U$ are affecting the bond-length disproportionation between the nickel sites. Our results show that structural parameters can be obtained that are in very good agreement with present experimental data, and that DFT+$U$ is in principle able to capture the most important structural trends across the nickelate series. However, the amplitude of the bond-length disproportionation depends very strongly on the specific value used for the Hubbard $U$ parameter and also on the type of magnetic order imposed in the calculation. Regarding the relative stability of different magnetic orderings, a realistic antiferromagnetic order, consistent with the experimental observations, is favored for small $U$ values, and becomes more and more favorable compared to the ferromagnetic state towards the end of the series (i.e., towards $R$=Pr). Nevertheless, it seems that the stability of the ferromagnetic state is generally overestimated within the DFT+$U$ calculations. Our work provides a profound starting point for more detailed experimental investigations, and also for future studies using more advanced computational techniques such as, e.g., DFT combined with dynamical mean-field theory.
Whilst electron correlations were previously recognized to trigger beyond conventional direct current (DC) electronic transportations (e.g. metal-to-insulator transitions, bad metal, thermistors), their respective influences to the alternation current (AC) transport are largely overlooked. Herein, we demonstrate active regulations in the electronic functionalities of d-band correlated rare-earth nickelate (ReNiO3) thin films, by simply utilizing their electronic responses to AC-frequencies (fAC). Assisted by temperature dependent near edge X-ray absorption fine structure analysis, we discovered positive temperature dependences in Coulomb viscosity of ReNiO3 that moderates their AC impedance. Distinguished crosslinking among R(Real)-fAC measured in nearby temperatures is observed that differs to conventional oxides. It enables active adjustability in correlated transports of ReNiO3, among NTCR-, TDelta- and PTCR- thermistors, via fAC from the electronic perspective without varying materials or device structures. The TDelta-fAC relationship can be further widely adjusted via Re composition and interfacial strains. The AC-frequency sensitivity discovered in ReNiO3 brings in a new freedom to regulating and switching the device working states beyond the present semiconductor technologies. It opens a new paradigm for enriching novel electronic applications catering automatic transmission or artificial intelligence in sensing temperatures and frequencies.
The acute sensitivity of the electrical resistance of certain systems to magnetic fields known as extreme magnetoresistance (XMR) has recently been explored in a new materials context with topological semimetals. Exemplified by WTe$_{2}$ and rare earth monopnictide La(Sb,Bi), these systems tend to be non-magnetic, nearly compensated semimetals and represent a platform for large magnetoresistance driven by intrinsic electronic structure. Here we explore electronic transport in magnetic members of the latter family of semimetals and find that XMR is strongly modulated by magnetic order. In particular, CeSb exhibits XMR in excess of $1.6 times 10^{6}$ % at fields of 9 T while the magnetoresistance itself is non-monotonic across the various magnetic phases and shows a transition from negative magnetoresistance to XMR with field above magnetic ordering temperature $T_{N}$. The magnitude of the XMR is larger than in other rare earth monopnictides including the non-magnetic members and follows an non-saturating power law to fields above 30 T. We show that the overall response can be understood as the modulation of conductivity by the Ce orbital state and for intermediate temperatures can be characterized by an effective medium model. Comparison to the orbitally quenched compound GdBi supports the correlation of XMR with the onset of magnetic ordering and compensation and highlights the unique combination of orbital inversion and type-I magnetic ordering in CeSb in determining its large response. These findings suggest a paradigm for magneto-orbital control of XMR and are relevant to the understanding of rare earth-based correlated topological materials.
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