Structurally triggered metal-insulator transition in rare-earth nickelates

Mercy, Alain; Bieder, Jordan; Íñiguez, Jorgé; Ghosez, Philippe

doi:10.1038/s41467-017-01811-x

Cited by 152 publications

(161 citation statements)

References 53 publications

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“…In Ref. [6], the unusual cooperative coupling of B oc with M z and R xy at the origin of this triggered mechanism was moreover traced back in the electronic properties of nickelates and further related to a type of structurally triggered Peierls instability. Fig 1g) shows that this explanation still hands for ferrites.…”

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confidence: 99%

“…On the one hand, RNiO 3 compounds show on cooling a MIT (T M IT = 0 − 600K) concomitant with a structural transition from Pbnm to P 2 1 /n [5]. This lowering of symmetry arises from the appearance of a breathing distortion of the oxygen octahedra (B oc ), recently assigned to a structurally triggered mechanism [6] and producing a kind of charge ordering (CO) [7][8][9][10]. On the other hand, RMnO 3 compounds also exhibit on cooling a MIT (T M IT ≈ 750K) but associated to orbital ordering (OO) and linked to the appearance of Jahn-Teller distortions (M JT ) compatible with the P bnm symmetry [11,12].…”

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From charge- to orbital-ordered metal-insulator transition in alkaline-earth ferrites

et al. 2018

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While CaFeO3 exhibits upon cooling a metal-insulator transition linked to charge ordering, SrFeO3 and BaFeO3 keep metallic behaviors down to very low temperatures. Moreover, alkaline-earth ferrites do not seem prone to orbital ordering in spite of the d 4 formal occupancy of Fe 4+ . Here, from first-principles simulations, we show that the metal-insulator transition of CaFeO3 is structurally triggered by oxygen rotation motions as in rare-earth nickelates. This not only further clarifies why SrFeO3 and BaFeO3 remain metallic but allows us to predict that an insulating charge-ordered phase can be induced in SrFeO3 from appropriate engineering of oxygen rotation motions. Going further, we unveil the possibility to switch from the usual charge-ordered to an orbital-ordered insulating ground state under moderate tensile strain in CaFeO3 thin films. We rationalize the competition between charge and orbital orderings, highlighting alternative possible strategies to produce such a change of ground state, also relevant to manganite and nickelate compounds.

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From charge- to orbital-ordered metal-insulator transition in alkaline-earth ferrites

et al. 2018

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“…For Mott insulators, this defines the field of Mottronics. This approach is especially suitable for the functionalization of giant conductivity variations across the metal-insulator transition (MIT) 10,11 , with the change driven by various mechanisms such as structural distortions 12 , substrate-induced strain 13 , thickness 14,15 , and bias 11 , as well as for the switching of the spin order between different magnetic ground states 9,16 .…”

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Electron-polaron dichotomy of charge carriers in perovskite oxides

et al. 2020

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Many transition metal oxides (TMOs) are Mott insulators due to strong Coulomb repulsion between electrons, and exhibit metal-insulator transitions (MITs) whose mechanisms are not always fully understood. Unlike most TMOs, minute doping in CaMnO 3 induces a metallic state without any structural transformations. This material is thus an ideal platform to explore band formation through the MIT. Here, we use angle-resolved photoemission spectroscopy to visualize how electrons delocalize and couple to phonons in CaMnO 3 . We show the development of a Fermi surface where mobile electrons coexist with heavier carriers, strongly coupled polarons. The latter originate from a boost of the electron-phonon interaction (EPI). This finding brings to light the role that the EPI can play in MITs even caused by purely electronic mechanisms. Our discovery of the EPI-induced dichotomy of the charge carriers explains the transport response of Ce-doped CaMnO 3 and suggests strategies to engineer quantum matter from TMOs.

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“…15 demonstrated failure to stabilize JT distortions in LaMnO3, again, in contradiction with both experiments and DMFT calculations. Such naïve (N-) DFT calculations, however, do not necessarily represent what proper DFT can do, as demonstrated in recent calculations for the binary 3d oxides MnO, NiO, CoO and FeO 16 or ABO3 materials [17][18][19][20][21][22][23][24] . In these calculations 16,24 , the PM phase, which is a…”

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Mott gapping in 3dABO3 perovskites without Mott-Hubbard interelectronic repulsion energy U

2019

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The existence of band gaps in Mott insulators such as perovskite oxides with partially filled 3d shells has been traditionally explained in terms of strong, dynamic inter-electronic repulsion codified by the on-site repulsion energy U in the Hubbard Hamiltonian. The success of the "DFT+U approach" where an empirical on-site potential term U is added to the exchange-and correlation Density Functional Theory (DFT) raised questions on whether U in DFT+U represents interelectronic correlation in the same way as it does in the Hubbard Hamiltonian, and if empiricism in selecting U can be avoided. Here we illustrate that ab-initio DFT without any U is able to predict gapping trends and structural symmetry breaking (octahedra rotations, Jahn-Teller modes, bond disproportionation) for all ABO3 3d perovskites from titanates to nickelates in both spin-ordered and spin disordered paramagnetic phases.We describe the paramagnetic phases as a supercell where individual sites can have different local environments thereby allowing DFT to develop finite moments on different sites as long as the total cell has zero moment. We use a recently developed exchange and correlation functional ("SCAN") that is sanctioned by the usual single-determinant, mean-field DFT paradigm with static correlations, but has a more precise rendering of self-interaction cancelation. Our results suggest that strong dynamic electronic correlations are not playing a universal role in gapping of 3d ABO3 Mott insulators, and opens the way for future applications of DFT for studying a plethora of complexity effects that depend on the existence of gaps, such as doping, defects, and band alignment in ABO3 oxides. ensuing localization. Within this framework, the experimental observations of a variety of different symmetry-breaking modes, such as those presented in Fig.1, or magnetic moments is not related to the gapping mechanism but can appear afterwards as an additional effect.Whereas Density Functional Theory (DFT) has been shown to be able to address numerous physical effects in such oxides, including ferroelectricity 10 , catalysis 11 and electrical battery voltage 12 , its use of a single Slater determinant and its mean-field treatment of electronelectron interactions (static correlations) has, according to numerous literature statements [13][14][15] , disqualified it for the study such "strongly correlated" oxides, requiring far more computationally costly dynamically correlated methodologies, such as Dynamical Mean Field Theory (DMFT). However, the DFT calculations in such demonstrations of failure 13-15 often used a nonspin polarized description and at times exchange correlation functionals that do not distinguish occupied from unoccupied orbitals (LDA or GGA functionals without U), and generally neglect sublattice displacements. For example, Ref. 14 demonstrated vanishing band gaps in LuNiO3, in contradiction with experiment, and Ref. 15 demonstrated failure to stabilize JT distortions in LaMnO3, again, in contradiction with both experiments and DMFT cal...

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Structurally triggered metal-insulator transition in rare-earth nickelates

Cited by 152 publications

References 53 publications

From charge- to orbital-ordered metal-insulator transition in alkaline-earth ferrites

From charge- to orbital-ordered metal-insulator transition in alkaline-earth ferrites

Electron-polaron dichotomy of charge carriers in perovskite oxides

Mott gapping in 3dABO3 perovskites without Mott-Hubbard interelectronic repulsion energy U

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