Summary
This study developed a megapascal-level high-pressure oxygen-assisted chemical synthesis route that successfully enabled the effective growth of infinite-layer nickelates extending to heavier rare earth elements, with composition (RE1-yRE'y)1-xEuxNiO2 (RE/RE': Pr, Nd, Sm, Gd, Dy). Hole doping was realized through Eu2+/Eu3+ valence variation. At the superconducting dome boundaries of Nd1-xEuxNiO2 and Pr1-xEuxNiO2 systems, robust uniaxial anisotropic magnetic-field reentrant superconductivity was observed, arising from the competition between Eu2+ 4f7 magnetic moments and magnetic fluctuations, while the optimally doped regions exhibited conventional high-temperature superconductivity with a critical current density reaching ~266 kA/cm2 at 2 K, surpassing that of traditional Sr/Ca-doped systems. Further introduction of different RE′ magnetic ions allowed tuning of the exchange field strength and thereby modulation of quantum criticality, both enhancing the reentrant behavior and elevating T_c to 40.1 K. This work reveals the critical role of rare-earth 4f magnetic moments in modulating pairing strength and quantum criticality, establishing a synthetic foundation for utilizing the infinite-layer nickelate platform to investigate 4f-related unconventional superconductivity and quantum phase transitions.
Materials
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Methods
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Keywords
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Highlights
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Conclusions
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Main claims
- A chemical avenue enables effective growth of (RE,RE')1-xEuxNiO2, revealing RE-4f-related quantum competition between high-Tc and reentrant superconductivity.
- Evidence: 'Herein, we open up chemical avenues to enable effective growth of (RE1-yRE'y)1-xEuxNiO2 (RE/RE': Pr, Nd, Sm, Gd, Dy), giving rise to discoveries of RE-4f-related quantum competition between high-Tc and reentrant superconductivity.' (Abstract)
- Robust magnetic-field-reentrant superconductivity with uniaxial anisotropy is observed at superconducting-dome boundaries, stemming from Eu2+-4f7 competition between magnetic-fluctuation promoted pairing and exchange-field interactions.
- Evidence: 'Robust magnetic-field-reentrant superconductivity with uniaxial anisotropy is observed at superconducting-dome boundaries, stemming from Eu2+-4f7 associated competition between magnetic-fluctuation promoted pairing and exchange-field interactions.' (Abstract)
- Quantum-criticality is further modulable via RE(RE')-magnetism, which either reinforces reentrancy or elevates Tc (40.1 K) with more robust critical-current-density (≈266 kA/cm2 at 2 K) beyond Sr-/Ca-doped counterparts.
- Evidence: 'Their quantum-criticality is further modulable via RE(RE')-magnetism, which either reinforces reentrancy or elevates Tc (40.1 K) with more robust critical-current-density (≈266 kA/cm2 at 2 K) beyond Sr-/Ca-doped counterparts.' (Abstract)
- Combining magneto-transport and LE-μSR unveils that strengthened Cooper pairing and promoted magnetic fluctuation via optimum Eu2+-4f7 interactions are responsible for elevated Tc and Jc beyond Sr/Ca systems.
- Evidence: 'Further introduction of different RE′ magnetic ions allowed tuning of the exchange field strength and thereby modulation of quantum criticality, both enhancing the reentrant behavior and elevating T_c to 40.1 K.' (Summary),'combining magneto-transport and LE-μSR measurements unveils the concomitant occurrence of strengthened Cooper pairing and promoted magnetic fluctuation' (Conclusion paraphrase)
Workflow
- Synthesis of infinite-layer nickelate thin films via high-pressure oxygen-assisted chemical route — Effective growth of (RE,RE')1-xEuxNiO2 infinite-layer nickelates with heavier rare-earths enabled by MPa-high-pO2 synthesis, overcoming thermodynamic limitations of vacuum epitaxy.
- Materials: RE(NO3)3; Ni(CH3COO)2; ethylene glycol monomethyl ether (EGME); NdGaO3 (110) substrate; CaH2
- Methods: spin coating; MPa-range high-pressure oxygen annealing; topotactic reduction with CaH2
- Observations: Perovskite precursor films exhibit metal-insulator transitions (T_MIT increasing with Eu content); XRD confirms transformation to infinite-layer structure after reduction; Cross-section STEM shows ≈20 nm thick films with coherent interfaces; some reduced crystallinity
- Transport measurements and superconducting phase diagram mapping — Robust magnetic-field-reentrant superconductivity with uniaxial anisotropy emerges at quantum boundaries of the superconducting dome, competing with high-Tc superconductivity, associated with Eu2+ 4f7 magnetic moments.
- Materials: Nd1-xEuxNiO2 films; Pr1-xEuxNiO2 films
- Methods: resistivity vs temperature under magnetic fields up to 35T; magnetic field-dependent resistivity mapping; critical current density measurements
- Observations: Optimum-doped Nd0.55Eu0.45NiO2 shows conventional superconductivity with Tc,onset ≈37.6 K, monotonically suppressed by field; Underdoped (x=0.2-0.3) and overdoped (x=0.52-0.6) samples exhibit field-reentrant superconductivity, zero resistance re-emerging at high fields; Phase diagrams reveal reentrance exclusively at superconducting dome boundaries; Jc reaches 266 kA/cm2 at 2 K for optimum doping, robust under 9 T field
- Modulation of reentrant behavior and Tc via rare-earth substitution — Quantum criticality between reentrant and high-Tc SC is tunable via RE' magnetism; Gd3+ (4f7) reinforces reentrancy via Jaccarino-Peter effect, while weak magnetic RE' mixing elevates Tc by disturbing spin ordering.
- Materials: (Nd1-yRE'y)0.65Eu0.35NiO2 with RE' = Pr, Sm, Gd, Dy
- Methods: same synthesis route; resistivity under magnetic field; angular-dependent magnetotransport
- Observations: Gd-substituted samples (y=0.05,0.1,0.2) show enhanced field-reentrant superconductivity; Dy, Pr, Sm show conventional SC; Angular mapping reveals uniaxial anisotropy with reentrant region near c-axis; Introducing RE' with reduced magnetism (Pr, Sm, mixed) elevates Tc up to 40.1K
- Muon spin spectroscopy and pairing mechanism investigation — Enhanced magnetic fluctuations and spin ordering at superconducting state in Eu-doped nickelates strengthen Cooper pairing, explaining elevated Tc and Jc beyond Sr/Ca-doped systems.
- Materials: Nd0.6Eu0.4NiO2 film on LSAT (100) substrate
- Methods: low-energy muon-spin spectroscopy (LE-μSR)
- Observations: Abrupt increase in ZF relaxation rate λ_ZF below Tc, to ≈2.5 μs-1, much larger than Sr-doped counterparts (0.22-0.48 μs-1); Stretch exponent β decreases to ≈0.5-0.6, indicating spin-glass-like state below Tc