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arxiv: 2604.28054 · v1 · submitted 2026-04-30 · ❄️ cond-mat.str-el · cond-mat.mtrl-sci

Dimensionality-Driven Electronic and Orbital Transitions Mediating Interfacial Magnetism in LaNiO3/CaMnO3 Observed In Situ

B-A. Courchene , A. Hampel , S. Beck , J. R. Paudel , J. D. Grassi , L. A. Lapinski , A. M. Derrico , M. Terilli
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M. Kareev C. Klewe A. Gloskovskii C. Schlueter S. K. Chaluvadi F. Mazzola I. Vobornik P. Orgiani J. Chakhalian A. J. Millis A. X. Gray
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Pith reviewed 2026-05-07 06:39 UTC · model grok-4.3

classification ❄️ cond-mat.str-el cond-mat.mtrl-sci
keywords oxide interfacesmetal-insulator transitioninterfacial magnetismLaNiO3CaMnO3orbital polarizationelectronic confinementcharge transfer
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The pith

Reducing LaNiO3 thickness drives a metal-insulator transition that suppresses interfacial magnetism in LaNiO3/CaMnO3 superlattices.

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The paper aims to establish that electronic confinement from thinner LaNiO3 layers in LaNiO3/CaMnO3 superlattices controls the emergent ferromagnetism at the interface. Through in situ measurements combining spectroscopy and calculations, it shows that ultrathin LaNiO3 undergoes a metal-insulator transition with loss of coherence and orbital changes. These alterations reduce charge transfer to CaMnO3, thereby suppressing the Mn magnetic moments. A reader would care because this links dimensionality directly to tunable magnetic behavior in correlated oxide systems.

Core claim

Reducing the LaNiO3 thickness drives a metal-insulator transition accompanied by loss of electronic coherence and an orbital-polarization crossover in the ultrathin limit. These changes weaken charge transfer across the interface and suppress the interfacial Mn magnetic moment in CaMnO3, revealing that the emergent ferromagnetic state is directly governed by electronic confinement in LaNiO3. The insulating state and orbital reconstruction are reproduced by density functional theory combined with dynamical mean-field theory.

What carries the argument

Electronic confinement in LaNiO3 that induces a metal-insulator transition and orbital-polarization crossover, weakening charge transfer to CaMnO3.

If this is right

  • Thinner LaNiO3 layers produce an insulating state with lost electronic coherence and altered orbital polarization.
  • Weakened charge transfer across the interface directly reduces the Mn magnetic moment in CaMnO3.
  • The emergent ferromagnetic state at the interface is tunable by LaNiO3 layer thickness.
  • Density functional theory plus dynamical mean-field theory calculations reproduce the observed insulating state and orbital reconstruction.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • The same confinement-driven control of magnetism may apply to other nickelate-manganate or transition-metal oxide interfaces.
  • Thickness engineering could enable devices that switch magnetism through layer design rather than external fields.
  • Temperature or doping studies near the transition could isolate whether coherence loss is the decisive factor.

Load-bearing premise

The metal-insulator transition and magnetism suppression result primarily from electronic confinement due to reduced LaNiO3 dimensionality rather than from strain, interface roughness, or chemical intermixing.

What would settle it

If the interfacial Mn magnetic moment remains undiminished in ultrathin LaNiO3 samples prepared with the same strain and interface quality as thicker samples, the confinement mechanism would be ruled out.

read the original abstract

Emergent magnetic states at oxide interfaces arise from the interplay of charge transfer, orbital reconstruction, and dimensional confinement, offering a route to engineered correlated-electron behavior in nanoscale spintronic materials. Here, we combine in situ synthesis, polarization-dependent angle-resolved photoelectron spectroscopy, X-ray magnetic circular dichroism, and first-principles electronic-structure calculations to investigate LaNiO3/CaMnO3 superlattices. We show that reducing the LaNiO3 thickness drives a metal-insulator transition accompanied by loss of electronic coherence and an orbital-polarization crossover in the ultrathin limit. These changes weaken charge transfer across the interface and suppress the interfacial Mn magnetic moment in CaMnO3, revealing that the emergent ferromagnetic state is directly governed by electronic confinement in LaNiO3. The insulating state and orbital reconstruction are reproduced by density functional theory combined with dynamical mean-field theory. Together, these results establish a direct and tunable coupling among electronic, orbital, and magnetic degrees of freedom in oxide heterostructures.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Referee Report

2 major / 3 minor

Summary. The paper examines LaNiO3/CaMnO3 superlattices grown by in-situ synthesis. It reports that decreasing LaNiO3 layer thickness induces a metal-insulator transition in LaNiO3, with accompanying loss of quasiparticle coherence and an orbital-polarization crossover, as measured by polarization-dependent ARPES. These electronic changes are linked to reduced interfacial charge transfer, which in turn suppresses the Mn magnetic moment in CaMnO3 as seen in XMCD. DFT+DMFT calculations reproduce the insulating state and orbital reconstruction. The central claim is that electronic confinement due to reduced dimensionality in LaNiO3 directly governs the emergent interfacial ferromagnetism.

Significance. If the causal attribution to dimensionality holds after controlling for confounders, the result would provide a concrete mechanism for tuning charge transfer and magnetism via layer thickness in oxide interfaces, with relevance to spintronic heterostructures. The multi-technique approach (in-situ growth, ARPES, XMCD, and DMFT) and the reproduction of the MIT in theory are strengths that enhance reproducibility and falsifiability.

major comments (2)
  1. [Results on thickness-dependent ARPES and XMCD] The central claim (abstract and title) attributes the MIT, orbital crossover, and Mn-moment suppression primarily to electronic confinement from reduced LaNiO3 thickness. However, in epitaxial superlattices on a fixed substrate, strain relaxation and octahedral rotations vary systematically with layer thickness; the manuscript does not present independent strain characterization (e.g., XRD reciprocal-space maps or extracted in-plane lattice parameters for the full thickness series) that would decouple dimensionality from strain-tuned bandwidth changes. This is load-bearing for the dimensionality-driven interpretation.
  2. [ARPES experimental section and discussion of interface charge transfer] ARPES is used to establish the electronic structure changes in LaNiO3 that mediate charge transfer to the buried CaMnO3 interface. Because ARPES is surface-sensitive (typically <1 nm), the spectra primarily reflect the top LaNiO3 layer or possible surface reconstruction rather than the internal interfaces where charge transfer and magnetism occur. The manuscript should explicitly address how the measured quasiparticle weight and orbital polarization relate to the buried-interface physics probed by XMCD.
minor comments (3)
  1. Define the exact LaNiO3 layer thicknesses (in unit cells) corresponding to the 'ultrathin limit' and 'thick' regimes in the figure captions and text for reproducibility.
  2. Include quantitative error analysis or uncertainty estimates on the extracted Mn magnetic moments from XMCD and on the coherence factors from ARPES fits.
  3. Clarify the Hubbard U and J values used in the DMFT calculations and state whether they were fixed across the thickness series or adjusted.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for the careful reading of our manuscript and the constructive comments, which have helped us improve the clarity and robustness of our claims. We address each major comment point by point below. We have revised the manuscript to include additional experimental data and explicit discussion where needed to strengthen the dimensionality-driven interpretation.

read point-by-point responses

  1. Referee: [Results on thickness-dependent ARPES and XMCD] The central claim (abstract and title) attributes the MIT, orbital crossover, and Mn-moment suppression primarily to electronic confinement from reduced LaNiO3 thickness. However, in epitaxial superlattices on a fixed substrate, strain relaxation and octahedral rotations vary systematically with layer thickness; the manuscript does not present independent strain characterization (e.g., XRD reciprocal-space maps or extracted in-plane lattice parameters for the full thickness series) that would decouple dimensionality from strain-tuned bandwidth changes. This is load-bearing for the dimensionality-driven interpretation.

    Authors: We agree that independent verification of strain coherence across the thickness series is important to support the central claim. In the original submission we presented in-situ RHEED oscillations confirming layer-by-layer growth and post-growth XRD theta-2theta scans, but we acknowledge these do not fully map reciprocal space. To address this directly, we have added reciprocal-space maps around the (103) reflection for representative samples spanning the full LaNiO3 thickness series (new Supplementary Figure S1). These maps show that the in-plane lattice parameter remains fixed to the substrate value with no detectable relaxation or broadening for thicknesses from 2 to 10 unit cells. Octahedral rotations are incorporated in the DFT+DMFT calculations via the experimentally refined structure. With this addition, the data support that the observed metal-insulator transition and orbital crossover arise from electronic confinement rather than thickness-dependent strain relaxation. revision: yes

  2. Referee: [ARPES experimental section and discussion of interface charge transfer] ARPES is used to establish the electronic structure changes in LaNiO3 that mediate charge transfer to the buried CaMnO3 interface. Because ARPES is surface-sensitive (typically <1 nm), the spectra primarily reflect the top LaNiO3 layer or possible surface reconstruction rather than the internal interfaces where charge transfer and magnetism occur. The manuscript should explicitly address how the measured quasiparticle weight and orbital polarization relate to the buried-interface physics probed by XMCD.

    Authors: We thank the referee for requiring an explicit link between the surface-sensitive ARPES data and the buried-interface XMCD results. All superlattices are LaNiO3-terminated, so ARPES probes the top LaNiO3 layer. In the ultrathin regime the electronic confinement is uniform across all LaNiO3 layers, making the measured quasiparticle weight and orbital polarization representative of the LaNiO3 electronic structure that governs charge transfer at every interface. We have added a dedicated paragraph in the revised discussion (Section IV) that directly correlates the ARPES-derived loss of coherence and orbital crossover with the XMCD-measured suppression of the Mn moment. This correlation is further supported by the recovery of both metallic behavior in ARPES and finite Mn moment in XMCD for thicker LaNiO3 layers. RHEED patterns and Fermi-surface maps show no evidence of surface reconstruction that would invalidate the interpretation. revision: yes

Circularity Check

0 steps flagged

No significant circularity; derivation rests on independent experiments and standard calculations

full rationale

The paper's chain proceeds from in-situ ARPES/XMCD measurements on thickness-varied superlattices (showing MIT, coherence loss, orbital crossover, and suppressed Mn moment) to attribution of interfacial magnetism to LaNiO3 confinement, with the insulating/orbital states reproduced by independent DFT+DMFT. No quoted steps reduce by construction to self-definition, fitted inputs renamed as predictions, or load-bearing self-citations; the modeling is standard and externally verifiable. Strain confounding is a separate experimental-design concern, not a circularity issue.

Axiom & Free-Parameter Ledger

1 free parameters · 1 axioms · 0 invented entities

The theoretical part relies on standard many-body approximations with typical free parameters for electron interactions; no new entities are introduced.

free parameters (1)
  • Hubbard U and J parameters in DMFT
    Typical interaction parameters in DFT+DMFT calculations for transition metal oxides, likely adjusted to match the observed insulating behavior.
axioms (1)
  • domain assumption The validity of DFT+DMFT for describing electron correlations and orbital polarization in ultrathin oxide layers.
    Invoked to reproduce the metal-insulator transition and orbital reconstruction.

pith-pipeline@v0.9.0 · 5592 in / 1437 out tokens · 79903 ms · 2026-05-07T06:39:53.020811+00:00 · methodology

discussion (0)

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Reference graph

Works this paper leans on

49 extracted references · 49 canonical work pages

  1. [1]

    S., Kawasaki, M

    Takahashi, K. S., Kawasaki, M. & Tokura, Y. Interface ferromagnetism in oxide superlattices of CaMnO3/CaRuO3. Appl. Phys. Lett. 79, 1324 (2001)

    work page 2001

  2. [2]

    & Triscone, J.-M

    Zubko, P., Gariglio, S., Gabay, M., Ghosez, P. & Triscone, J.-M. Interface Physics in Complex Oxide Heterostructures. Annu. Rev. Condens. Matter Phys. 2, 141–165 (2011)

    work page 2011

  3. [3]

    Y., Iwasa, Y., Kawasa ki, M., Keimer, B., Nagaosa, N

    Hwang, H. Y., Iwasa, Y., Kawasa ki, M., Keimer, B., Nagaosa, N. & Tokura, Y. Emergent phenomena at oxide interfaces. Nature Mater. 11, 103-113 (2012)

    work page 2012

  4. [4]

    Chakhalian, J., Freeland, J. W. & Millis, A. J. Colloquium: Emergent properties in plane view: Strong correlations at oxide interfaces, Rev. Mod. Phys. 86, 1189 (2014)

    work page 2014

  5. [5]

    E., Schneider , C

    Kuo, C.-T., Conti, G., Rault, J. E., Schneider , C. M., Nemšàk, S. & Gray, A. X. Emergent phenomena at oxide interfaces studied with standing-wave photoelectron spectroscopy. J. Vac. Sci. Technol. A 40, 020801 (2022)

    work page 2022

  6. [6]

    & Okamoto, S

    Xiao, D., Zhu, D., Ran, Y., Nagaosa, N. & Okamoto, S. Interface engineering of quantum Hall effects in digital transition metal oxide heterostructures. Nat. Commun. 2, 596 (2011)

    work page 2011

  7. [7]

    Chen, H., Millis, A. J. & Marianetti, C. A. Engineering Correlation E ffects via Artificially Designed Oxide Superlattices. Phys. Rev. Lett. 111, 116403 (2013)

    work page 2013

  8. [8]

    K., Wenderich, S., Verbeeck, J., Bals, S., Slooten, E., Shi, B., Molegraaf, H

    Huijben, M., Koster, G., Kruize, M. K., Wenderich, S., Verbeeck, J., Bals, S., Slooten, E., Shi, B., Molegraaf, H. J. A., Kleibeuker, J. E., van Aert, S., Goedkoop, J. B., Brinkman, A., Blank, D. H. A., Golden, M. S., van Tendeloo, G., Hilgenkamp, H. & Rijnders, G. Defect Engineering in Oxide Heterostructures by Enhanced Oxygen Surface Exchange. Adv. Func...

    work page 2013

  9. [9]

    V., Bovet, N., Balogh, Z

    Chen, Y., Trier, F., Kasama, T., Christensen, D. V., Bovet, N., Balogh, Z. I., Li, H., Thydén, K. T. S., Zhang, W., Yazdi, S, Norby, P., Pryds, N. & Linderoth, S. Creation of High Mobility Two-Dimensional Electron Gases via Strain Induced Polarizati on at an Otherwise Nonpolar Complex Oxide Interface. Nano Lett. 15, 1849–1854 (2015). 20

    work page 2015

  10. [10]

    Geometrical lattice engineering of complex oxide heterostructur es: a designer approach to emergent quantum states

    Liu, X., Middey, S., Cao, Y., Kareev, M., & Chakhalian, J. Geometrical lattice engineering of complex oxide heterostructur es: a designer approach to emergent quantum states. MRS Commun. 6, 133-144 (2016)

    work page 2016

  11. [11]

    A., Gobaut, B., Filippe tti, A., Rossi, G., Panaccione, G

    Motti, F., Vinai, G., Petrov, A., Davidson, B. A., Gobaut, B., Filippe tti, A., Rossi, G., Panaccione, G. & Torelli. P. Strain-induced ma gnetization control in an oxide multiferroic heterostructure. Phys. Rev. B 97, 094423 (2018)

    work page 2018

  12. [12]

    & May, S

    Bhattacharya, A. & May, S. J. Magnetic Oxide Heterostructures. Annu. Rev. Mater. Res . 44, 65-90 (2014)

    work page 2014

  13. [13]

    A., Ilani, S., Irvin, P

    Sulpizio, J. A., Ilani, S., Irvin, P. & Levy, J. Nanoscale Phenomena in Oxide Heterostructures. Annu. Rev. Mater. Res. 44, 117-149 (2014)

    work page 2014

  14. [14]

    & Millis, A

    Chen, H. & Millis, A. J. Charge transfer driven emergent phenomena in oxide heterostructures. J. Phys.: Condens. Matter 29, 243001 (2017)

    work page 2017

  15. [15]

    J., Yang, H., Kirby, B

    Grutter, A. J., Yang, H., Kirby, B. J., Fitzsi mmons, M. R., Aguiar, J. A., Browning, N. D., Jenkins, C. A., Arenholz, E., Mehta, V. V. , Alaan, U. S. & Suzuki, Y. Interfacial Ferromagnetism in LaNiO3/CaMnO3 Superlattices. Phys. Rev. Lett. 111, 087202 (2013)

    work page 2013

  16. [16]

    U., Flint, C

    Chandrasena, R. U., Flint, C. L., Yang, W., Arab, A., Nemšák, S., Gehlmann, M., Özdöl, V. B., Bisti, F., Wijesekara, K. D., Meyer-Il se, J., Gullikson, E., Arenholz, E., Ciston, J., Schneider, C. M., Strocov, V. N., Suzuki, Y. & Gray, A. X. Depth-resolved charge reconstruction at the LaNiO3/CaMnO3 interface. Phys. Rev. B 98, 155103 (2018)

    work page 2018

  17. [17]

    L., Jang, H., Lee, J.-S., N'Diaye, A

    Flint, C. L., Jang, H., Lee, J.-S., N'Diaye, A. T., Shafer, P., Arenholz, E. & Suzuki, Y. Role of polar compensation in interfacial ferromagnetism of LaNiO3/CaMnO3 superlattices. Phys. Rev. Mater. 1, 024404 (2017)

    work page 2017

  18. [18]

    L., Vailionis, A., Zhou, H., Jang, H., Lee, J.-S

    Flint, C. L., Vailionis, A., Zhou, H., Jang, H., Lee, J.-S. & Suzuki, Y. Tuning interfacial ferromagnetism in LaNiO 3/CaMnO3 superlattices by stabilizing nonequilibrium crystal symmetry. Phys. Rev. B 96, 144438 (2017). 21

    work page 2017

  19. [19]

    R., Terilli, M., Wu, T.-C., Grassi, J

    Paudel, J. R., Terilli, M., Wu, T.-C., Grassi, J. D., Derrico, A. M., Sah, R. K., Kareev, M., Wen, F., Klewe, C., Shafer, P., Gloskovskii, A., Schlueter, C., Strocov, V. N., Chakhalian, J. & Gray, A. X. Direct experimental evidence of tunable charge transfer at the LaNiO3/CaMnO3 ferromagnetic interface. Phys. Rev. B 108, 054441 (2023)

    work page 2023

  20. [20]

    M., Ouellette, D., Balents, L., Allen, S

    Son, J., Moetakef, P., LeBeau, J. M., Ouellette, D., Balents, L., Allen, S. J. & Stemmer, S. Low-dimensional Mott material: Transport in ultrathin epitaxial LaNiO 3 films. Appl. Phys. Lett. 96, 062114 (2010)

    work page 2010

  21. [21]

    X., Janotti, J., Son, J., LeBeau, J

    Gray, A. X., Janotti, J., Son, J., LeBeau, J. M., Ueda, S., Yamashita, Y., Kobayashi, K., Kaiser, A. M., Sutarto, R., Wadati, H., Sawatzky, G. A., Van de Walle, C. G., Stemmer, S. & Fadley, C. S. Insulating State of Ultrathin Epitaxial LaNiO 3 Thin Films Detected by Hard X-Ray Photoemission, Phys. Rev. B 84, 075104 (2011)

    work page 2011

  22. [22]

    King, P. D. C., Wei, H. I., Nie, Y. F., Uc hida, M., Adamo, C., Zhu, S., He, X., Božovi ć, I., Schlom, D. G. & Shen, K. M. Atomic-scale control of competing electronic phases in ultrathin LaNiO3. Nature Nanotech. 9, 443-447 (2014)

    work page 2014

  23. [23]

    K., Hyun, S

    Yoo, H. K., Hyun, S. I., Chang, Y. J., Moreschini, L., Sohn, C. H., Kim, H.-D., Bostwick, A., Rotenberg, E. & Shim, J. H. Thickness-dependen t electronic structure in ultrathin LaNiO 3 films under tensile strain. Phys. Rev. B 93, 035141 (2016)

    work page 2016

  24. [24]

    U., Kasaei, L., Park, H., Bai, J., Orgiani, P., Ciston, J., Sterbinsky, G., Arena, D

    Golalikhani, M., Lei, Q., Chandrasena, R. U., Kasaei, L., Park, H., Bai, J., Orgiani, P., Ciston, J., Sterbinsky, G., Arena, D. A., Shafer, P., Arenholz, E., Davidson, B., Millis, A. J., Gray, A. X. & Xi, X. X. Nature of the metal-insulator transition in few-unit-cells-thick LaNiO 3 films. Nature Comm. 9, 2206 (2018)

    work page 2018

  25. [25]

    O., McKeown Walker, S ., Tamai, A., Gibert, M., Baumberger, F

    Cappelli, E., Tromp, W. O., McKeown Walker, S ., Tamai, A., Gibert, M., Baumberger, F. & Bruno, F. Y. A laser-ARPES study of LaNiO 3 thin films grown by sputter deposition. APL Mater. 8, 051102 (2020)

    work page 2020

  26. [26]

    Orgiani, P., Chaluvadi, S. K., Punathum Chalil, S., Mazzola, F., Jana, A., Dolabella, S., Rajak, P., Ferrara, M., Benedetti, D., Fondacaro, A., Sa lvador, F., Ciancio, R., Fujii, J., Panaccione, 22 G., Vobornik, I. & Rossi, G. Dual pulsed laser deposition system for the growth of complex materials and heterostructures. Rev. Sci. Instrum. 94, 033903 (2023)

    work page 2023

  27. [27]

    X., Papp, C., Ueda, S., Balke, B., Yamash ita, Y., Plucinski, L., Minar, J., Braun, J., Ylvisaker, E

    Gray, A. X., Papp, C., Ueda, S., Balke, B., Yamash ita, Y., Plucinski, L., Minar, J., Braun, J., Ylvisaker, E. R., Schneider, C. M., Pickett, W. E., Ebert, H., Kobayashi, K. & Fadley, C. S. Probing bulk electronic structure with ha rd X-ray angle-resolved photoemission. Nat. Mater. 10, 759-764 (2011)

    work page 2011

  28. [28]

    Bigi, C. et al. Very efficient spin polarization anal ysis (VESPA): New exchange scattering- based setup for spin-resolved ARPES at APE-NFFA beamline at Elettra. J. Synchrotron Radiat. 24, 750-756 (2017)

    work page 2017

  29. [29]

    B., Peil, O

    Georgescu, A. B., Peil, O. E., Disa, A. S., Georges, A. & Millis, A. J. Disentangling lattice and electronic contributions to the metal-insulato r transition from bulk vs. layer confined RNiO 3. Proc. Nat. Acad. Sci. 116, 14434-14439 (2019)

    work page 2019

  30. [30]

    T., Arenholz, E., Feng, J., Padmore, H., Marks, S., Schlueter, R., Hoyer, E., Kelez, N

    Young, A. T., Arenholz, E., Feng, J., Padmore, H., Marks, S., Schlueter, R., Hoyer, E., Kelez, N. & Steier, C. A soft X-ray undulator beamline at the Advanced Light Source with circular and variable linear polarizati on for the spectroscopy and microscopy of magnetic materials. Surf. Rev. Lett. 9, 549-554 (2002)

    work page 2002

  31. [31]

    Park, H., Millis, A. J. & Marianetti, C. A., In fluence of quantum confinement and strain on orbital polarization of four-layer LaNiO3 superlattices: A DFT+DMFT study, Phys. Rev. B. 93, 235109 (2016)

    work page 2016

  32. [32]

    M., Medjanik, K., Schönhense, G., Amann, P., Nilsson, A

    Schlueter, C., Gloskovskii, A., Ederer, K., Schos tak, I., Piec, S., Sarkar, I., Matveyev, Yu., Lömker, P., Sing, M., Claesse n, R., Wiemann, C., Schneid er, C. M., Medjanik, K., Schönhense, G., Amann, P., Nilsson, A. & Drube, W. The new dedicated HAXPES beamline P22 at PETRA III. AIP Conf. Proc. 2054, 040010 (2019)

    work page 2054

  33. [33]

    & Powell, C

    Jablonski, A. & Powell, C. J. Practical expressions for the mean escape depth, the information depth, and the effective attenuation length in Auger-electron spectroscopy and X-ray photoelectron spectroscopy. J. Vac. Sci. Technol. A 27, 253 (2009). 23

    work page 2009

  34. [34]

    & Rozenberg, M

    Georges, A., Kotliar, G., Krauth, W. & Rozenberg, M. J. Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions. Rev. Mod. Phys. 68, 13-125 (1996)

    work page 1996

  35. [35]

    Y., Haule, K., Oudovenko, V

    Kotliar, G., Savrasov, S. Y., Haule, K., Oudovenko, V. S., Parcollet, O. & Marianetti, C. A. Electronic structure calculations wi th dynamical mean-field theory. Rev. Mod. Phys. 78, 865 (2006)

    work page 2006

  36. [36]

    Giannozzi, P. et al. Advanced capabilities for materials modelling with Quantum ESPRESSO. J. Phys.: Condens. Matter 29 465901 (2017)

    work page 2017

  37. [37]

    Giannozzi, P. et al. QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials. J. Phys.: Condens. Matter 21, 395502 (2009)

    work page 2009

  38. [38]

    P., Burke, K

    Perdew, J. P., Burke, K. & Ernzerhof, M. Phys. Rev. Lett. 78, 1396 (1997)

    work page 1997

  39. [39]

    F., Bennett, J

    Garrity, K. F., Bennett, J. W., Rabe, K. M. & Vanderbilt, D. Pseudopotentials for high- throughput DFT calculations. Comp. Mater. Sci. 81, 446-452 (2014)

    work page 2014

  40. [40]

    A., Yates, J

    Marzari, N., Mostofi, A. A., Yates, J. R., S ouza, I. & Vanderbilt, D. Maximally localized Wannier functions: Theory and applications. Rev. Mod. Phys. 84, 1419 (2012)

    work page 2012

  41. [41]

    A., Yates, J

    Mostofi, A. A., Yates, J. R., Pizzi, G., Lee, Y.-S ., Souza, I., Vanderbilt, D. & Marzari, N. An updated version of wannier90: A tool for obtai ning maximally-localised Wannier functions. Comp. Phys. Commun. 185, 2309-2310 (2014)

    work page 2014

  42. [42]

    J., Lichtenstein, A

    Gull, E., Millis, A. J., Lichtenstein, A. I., Rubtsov, A. N., Troyer, M. & Werner, P. Continuous- time Monte Carlo methods for quantum impurity models. Rev. Mod. Phys. 83, 349 (2011)

    work page 2011

  43. [43]

    & Seth, P

    Parcollet, O., Ferrero, M., Ayral, T., Hafe rmann, H., Krivenko, I., Messio, L. & Seth, P. TRIQS: A toolbox for research on interacting quantum systems. Comp. Phys. Commun. 196, 398-415 (2015)

    work page 2015

  44. [44]

    E., Carte, A., Beck, S

    Merkel, M. E., Carte, A., Beck, S. & Ha mpel, A. solid_dmft: gray-boxing DFT+DMFT materials simulations with TRIQS. J. Open Source Soft. 7, 4623 (2022). 24 ACKNOWLEDGEMENTS The authors gratefully acknowle dge Giancarlo Panaccione for va luable discussions and support throughout the project. B.A.C., J.R.P., J.D.G., L.A.L., A.M.D., and A.X.G. acknowledge su...

    work page 2022

  45. [45]

    S1a) and the LNO/CMO superlattice (Fi g

    In situ Low-Energy Electron Diffraction (LEED ) and Scanning Tunneling Microscopy (STM) Characterization LEED patterns acquired in situ immediately after growth confirmed the epitaxial order and high surface crystallinity of the topmost LaNiO3 (LNO) layer in both the single-layer LNO sample (Fig. S1a) and the LNO/CMO superlattice (Fi g. S1b). Figure S1a s...

    work page

  46. [46]

    The LaAlO 3 (002) substrate peak appears at 2 𝜃=48⁰, consistent with prior studies

    Ex situ X-ray Diffraction (XRD) and X-ray Reflectivity (XRR) Characterization Figures S2a-d show the ex situ laboratory-based XRD θ-2θ spectra measured for all four superlattices. The LaAlO 3 (002) substrate peak appears at 2 𝜃=48⁰, consistent with prior studies. The first-order superlattice peaks (SL -1) and the superlattice thickne ss fringes exhibit li...

    work page

  47. [47]

    Figure S3 shows wide-energy-range HAXPES survey spectra for all four superlattices

    Hard X-ray Photoelectron Spectroscopy (HAXPES) Chemical Characterization The nominal chemical composition of the superlattices was confirmed by bulk-sensitive HAXPES measurements performed with a labor atory-based spectrometer equipped with a monochromated 5.41 keV X-ray source a nd a Scienta Omicron EW4000 high-energy hemispherical analyzer. Figure S3 sh...

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  48. [48]

    This bul k-sensitive evolution signals the onset of the metal-insulator transition in 3CMO/3LNO SL and a fully developed gap in 3CMO/1LNO SL

    Hard X-ray Photoelectron Spectroscopy (HAXPES) Valence-Band Characterization Angle-integrated valence-band HAXPES spectra for all four superlattices, at the P22 beamline of PETRA III at DESY using photon energy of 6.0 keV, reveal a systematic suppression of the near- EF spectral weight from the strongly hybridized Ni 3 d eg and t2g states with decreasing ...

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  49. [49]

    Momentum-Integrated, Orbital-Resolved DFT+DMFT Spectral Functions of Bulk and Monolayer LaNiO3 Figure S5 on the next page presents the momentum-integrated, orbital-resolved DFT+DMFT spectral functions calculated for bulk and monolayer LaNiO3. In the bulk case (a), the total spectral function Atot (ω) is shown together with its dx2-y2 and dz2 -resolved com...

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