Spectroscopic comprehension of Mott-Hubbard insulator to negative charge transfer metal transition in 
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 thin films

Jana, Anupam; Sahoo, Sophia; Chowdhury, Sourav; Mandal, Arup Kumar; Choudhary, R. J.; Phase, D. M.; Raychaudhuri, A. K.

doi:10.1103/physrevb.106.205123

Cited by 11 publications

(6 citation statements)

References 67 publications

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“…Another feature within the 536-538 eV range suggests the O 2p-La 3d/Sr 3d hybridized state, while higher energy features are attributed to the O 2p-Co 4sp/4s and O 2p-Mn 4sp/4s hybridized regions. 32,33,34 Mn L3,2-edge XAS (Fig. 3b) show mixed-valence Mn 3+/4+ consistent with stoichiometric single layer LSMO films 35 and with more prominence of Mn 4+ state in BL1 (Supplementary Note I).…”

Section: Resultsmentioning

confidence: 56%

“…17). This unusual interfacial antiferromagnetic Mn/Co ordering in lieu of vivid ferromagnetism of the BLs are further confirmed through Goodenough-Kanamori-Anderson (GKA) rules 33,34 . According to the GKA rules, the Mn d3z 2 -r 2 -(O 2pzz)-Co dyz and Mn d3z 2 -r 2 -(O 2pzz)-Co dzx interactions in the BLs are antiferromagnetic in nature (Supplementary Figs.…”

Section: Resultsmentioning

confidence: 61%

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A new pathway to correlate the octahedral tilt coupling and spin-orbit reconstruction at oxide interfaces

DAS,

Dey,

Jagadish

et al. 2024

Preprint

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The direct experimental probing and detailed imaging of octahedral tilt, along with the control of magnetic ground state and spin-orbit occupancies in an artificially engineered heterointerface through the manipulation of strain via interface engineering, is the long-standing challenging issue addressed in this study. We introduce a novel methodology that involves the measurement of the projected O-O-O angles (OOOproj) between the neighboring in-plane BO6 octahedra of perovskite oxide (ABO3), demonstrating a precise quantification of strain-manipulated octahedral tilt in atomically engineered La0.7Sr0.3MnO3 (LSMO)/LaCoO3 (LCO) bilayer interfaces. The pronounced octahedral tilt on SrTiO3 (STO) substrate (under tensile strain) compared to LaAlO3 (LAO) substrate (under compressive strain) correlates with the enhanced (suppressed) magnetism under tensile (compressive) strain in bilayer configuration, especially within the framework of bond angle geometry and spin-charge-orbital reconstructions, contrasting with strain effects reported on individual single-phase films. Interfacial orbital reconstruction, Co/Mn antiferromagnetic coupling and their manipulation under strain are quantified through X-ray linear dichroism (XLD) and X-ray magnetic circular dichroism (XMCD) measurements, further confirmed by both molecular orbital theory and Goodenough-Kanamori-Anderson rules. First principles calculations unveil a higher (lower) magnetic moment of individual magnetic atoms with tensile (compressive) strain, while also explaining the unusual interfacial antiferromagnetism arising from the interplay of out-of-plane and in-plane d-orbital occupations, and the role of bond angle geometry. This endeavor paves a potential method to manipulate the octahedral tilt and resultant perturbed crystal field energy to explore and tailor emergent phenomena at heterointerfaces via atomically precise strain-interface engineering.

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Section: Resultsmentioning

confidence: 56%

Section: Resultsmentioning

confidence: 61%

A new pathway to correlate the octahedral tilt coupling and spin-orbit reconstruction at oxide interfaces

DAS,

Dey,

Jagadish

et al. 2024

Preprint

Self Cite

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“…Along these lines it has previously been shown that LaV 1− x Ni x O 3 transforms from Mott ( x = 0.0) to a charge-transfer insulator ( x = 0.8). 19…”

Section: Resultsmentioning

confidence: 99%

Tunable bandgaps in self-assembled transition metal-incorporated heterometallic M₂Sb₄ (M = V, Mn, Co, Ni, and Cu) oxo clusters

Navaneetha,

Ugandhar,

Samuel

et al. 2023

Dalton Trans.

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“…S2 b of SM 54 . Although N K-edge XAS has been used for the CB mapping, it does not reflect the true DOS of the transition-metal states, rather reflecting the N 2 projected metal 3 DOS 55 – 57 . Hence, N K-edge XAS is used here as a CB (see Fig.…”

Section: Resultsmentioning

confidence: 99%

Electronic correlations in epitaxial CrN thin film

Kalal,

Nayak,

Sahoo

et al. 2023

Sci Rep

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Chromium nitride (CrN) spurred enormous interest due to its coupled magnetostructural and unique metal-insulator transition. The underneath electronic structure of CrN remains elusive. Herein, the electronic structure of epitaxial CrN thin film has been explored by employing resonant photoemission spectroscopy (RPES) and X-ray absorption near edge spectroscopy study in combination with the first-principles calculations. The RPES study indicates the presence of a charge-transfer screened 3$$d ^n{\underline{L}}$$ d n L ̲ ($$L$$ L : hole in the N-2$$p$$ p ) and 3$$d ^{n-1}$$ d n - 1 final-states in the valence band regime. The combined experimental electronic structure along with the orbital resolved electronic density of states from the first-principles calculations reveals the presence of Cr(3$$d$$ d )-N(2$$p$$ p ) hybridized (3$$d ^n{\underline{L}}$$ d n L ̲ ) states between lower Hubbard (3$$d ^{n-1}$$ d n - 1 ) and upper Hubbard (3$$d ^{n+1}$$ d n + 1 ) bands with onsite Coulomb repulsion energy (U) and charge-transfer energy ($$\Delta$$ Δ ) estimated as $$\approx$$ ≈ 4.5 and 3.6 eV, respectively. It verifies the participation of ligand (N-2$$p$$ p ) states in low energy charge fluctuations and provides concrete evidence for the charge-transfer ($$\Delta<$$ Δ < U) insulating nature of CrN thin film.

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Spectroscopic comprehension of Mott-Hubbard insulator to negative charge transfer metal transition in LaNixV1−xO3 thin films

Cited by 11 publications

References 67 publications

A new pathway to correlate the octahedral tilt coupling and spin-orbit reconstruction at oxide interfaces

A new pathway to correlate the octahedral tilt coupling and spin-orbit reconstruction at oxide interfaces

Tunable bandgaps in self-assembled transition metal-incorporated heterometallic M₂Sb₄ (M = V, Mn, Co, Ni, and Cu) oxo clusters

Electronic correlations in epitaxial CrN thin film

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Spectroscopic comprehension of Mott-Hubbard insulator to negative charge transfer metal transition in LaNixV1−xO3 thin films

Cited by 11 publications

References 67 publications

A new pathway to correlate the octahedral tilt coupling and spin-orbit reconstruction at oxide interfaces

A new pathway to correlate the octahedral tilt coupling and spin-orbit reconstruction at oxide interfaces

Tunable bandgaps in self-assembled transition metal-incorporated heterometallic M2Sb4 (M = V, Mn, Co, Ni, and Cu) oxo clusters

Electronic correlations in epitaxial CrN thin film

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Tunable bandgaps in self-assembled transition metal-incorporated heterometallic M₂Sb₄ (M = V, Mn, Co, Ni, and Cu) oxo clusters