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Resolving Structural Origins for Superconductivity in Strain-Engineered La$_3$Ni$_2$O$_7$ Thin Films
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abstract
The discovery of high-temperature superconductivity in bulk La$_3$Ni$_2$O$_7$ under high hydrostatic pressure and, more recently, biaxial compression in epitaxial thin films has ignited significant interest in understanding the interplay between atomic and electronic structure in these compounds. Subtle changes in the nickel-oxygen bonding environment are thought to be key drivers for stabilizing superconductivity, but specific details of which bonds and which modifications are most relevant remains so far unresolved. While direct, atomic-scale structural characterization under hydrostatic pressure is beyond current experimental capabilities, static stabilization of strained La$_3$Ni$_2$O$_7$ films provides a platform well-suited to investigation with new picometer-resolution electron microscopy methods. Here, we use multislice electron ptychography to directly measure the atomic-scale structural evolution of La$_3$Ni$_2$O$_7$ thin films across a wide range of biaxial strains tuned via substrate. By resolving both the cation and oxygen sublattices, we study strain-dependent evolution of atomic bonds, providing the opportunity to isolate and disentangle the effects of specific structural motifs for stabilizing superconductivity. We identify the lifting of crystalline symmetry through modification of the nickel-oxygen octahedral distortions under compressive strain as a key structural ingredient for superconductivity. Rather than previously supposed $c$-axis compression, our results highlight the importance of in-plane biaxial compression in superconducting thin films, which suggests an alternative -- possibly cuprate-like -- understanding of the electronic structure. Identifying local regions of inhomogeneous oxygen stoichiometry and high internal strain near crystalline defects, we suggest potential pathways for improving the sharpness and temperature of the superconducting transition.
Forward citations
Cited by 19 Pith papers
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Orbital-Selective Diagonal-Gap Test of Pairing in La$_3$Ni$_2$O$_7$
Symmetry analysis shows orbital hybridization vanishes along the BZ diagonal, allowing the gap on alpha/beta pockets to test d_x2-y2 vs d_z2 dominance; experiments and RPA favor Hund's rule mechanism with full gap.
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Structural symmetry effects on the competition of density waves and superconductivity in bilayer nickelates
fRG calculations on bilayer nickelate models show that approaching the tetragonal limit makes SDW fluctuations degenerate, frustrating magnetic order and enhancing superconductivity, identifying lattice symmetry as th...
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Density waves in low-pressure bilayer nickelates
Unrestricted Hartree-Fock calculations show the second density-wave transition in La3Ni2O7 originates from double-stripe spin order becoming unstable toward a commensurate charge-density wave, yielding intertwined spi...
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Pressure-induced superconductivity in epitaxially-stabilized Pr$_3$Ni$_2$O$_7$ films
Epitaxially stabilized Pr3Ni2O7 films show pressure-induced superconductivity with onset Tc of 66 K at 22 GPa, while the Nd analog does not superconduct in the accessed pressure range.
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Nature of magnetism in bilayer nickelate La3Ni2O7 single crystals
Single-crystal neutron scattering establishes stripe antiferromagnetic order with strong interlayer coupling and competing in-plane exchanges in La3Ni2O7, yielding fluctuating moments comparable to cuprates but with l...
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Interlayer hybridization enables superconductivity in bilayer nickelates
Superconductivity in bilayer nickelates emerges only when coherent interlayer d_z2-p_z-d_z2 hybridization develops, suppressing static spin-density-wave order and damping spin excitations.
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Tunable superconductivity and spin density wave in La3Ni2O7/LaAlO3 thin films
Varying the Ni-Ni interlayer distance switches La3Ni2O7/LaAlO3 films between C-type and G-type spin density waves, with s± superconductivity emerging in between.
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Superexchanges and Charge Transfer in the La$_3$Ni$_2$O$_7$ Thin Films
In La3Ni2O7 thin films, the interlayer d3z2-r2 antiferromagnetic coupling is about 27% weaker than in bulk, in-plane coupling is nearly unchanged, and hole/electron doping is particle-hole asymmetric.
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Role of correlations in Ruddlesden-Popper bilayer nickelates under compressive strain
At -2% compressive strain, dynamic electron correlations make a dz2-derived flat band cross the Fermi level in bilayer La3Ni2O7, creating an extra Fermi pocket absent in static DFT+U; at -3% the pocket disappears.
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Pairing symmetry and superconductivity in La$_3$Ni$_2$O$_7$ thin films
RMFT on the bilayer two-orbital t-J model predicts s±-wave pairing in La3Ni2O7 thin films, with a nodeless beta pocket and Tc near 60 K, plus an inter-orbital d-wave channel that reinforces the dominant pairing.
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Theoretical study on ambient pressure superconductivity in La$_3$Ni$_2$O$_7$ thin films : structural analysis, model construction, and robustness of $s\pm$-wave pairing
s±-wave pairing in La3Ni2O7 thin films is robust across different crystal structures, and the halved transition temperature is reproduced only when the experimentally determined structure with small interlayer hopping...
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Optical control of the crystal structure in the bilayer nickelate superconductor La3Ni2O7 via nonlinear phononics
First-principles calculation shows selective excitation of an IR phonon mode in La3Ni2O7 produces a small nonlinear shift that moves the Ni-O-Ni bond angle closer to 180 degrees.
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Electronic theory for scanning tunneling microscopy spectra in bilayer nickelate thin films
Position-dependent STM spectra in La2PrNi2O7 are computed from a two-orbital bilayer model, showing orbital-selective coherence peaks and impurity scattering that enable band identification.
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Strain-Engineered Electronic Structure and Superconductivity in La$_3$Ni$_2$O$_7$ Thin Films
DFT-based tight-binding models and FRG calculations predict that reducing in-plane lattice constant or increasing out-of-plane constant in La3Ni2O7 films increases Fermi-level DOS and enhances Tc while preserving s± pairing.
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Theoretical study on ambient pressure superconductivity in La$_3$Ni$_2$O$_7$ thin films : structural analysis, model construction, and robustness of $s\pm$-wave pairing
s±-wave pairing remains robust in La3Ni2O7 thin-film models under FLEX, but reduced Tc is reproduced only when using the experimental structure's small interlayer hopping.
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Magnetic configurations and excitations in high-$T_{c}$ multilayer nickelates
Multi-orbital Hartree-Fock calculations identify single-stripe magnetic order in bilayers and mirror-odd SDW in trilayers as consistent with experimental magnetic excitations in multilayer nickelates.
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Squeezing dynamical singlets in bilayer nickelates
Dynamical singlets from 3z²-r² orbitals hybridized with x²-y² orbitals control the distinct pressure versus strain responses in bilayer nickelates.
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Superconductivity in bilayer La$_3$Ni$_2$O$_7$: A review focusing on the strong-coupling Hund's rule assisted pairing mechanism
Superconductivity in La3Ni2O7 arises from interlayer Cooper pairs of 3d_x2-y2 electrons driven by effective J_perp from Hund-assisted AFM exchange transfer, while localized 3d_z2 electrons form rung singlets that prod...
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Recent progress in nickelate superconductors
A comprehensive review of nickelate superconductors that surveys the 112, 327, and 43(10) families and frames the key open questions about their pairing mechanisms.
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