Summary
The research team conducted electrical transport measurements on (La, Pr, Sm)3Ni2O7 double-layer nickelate thin films and discovered a time-reversal symmetry breaking superconducting state accompanied by electronic glass behavior. This superconducting state emerges in the low-temperature regime near zero resistance, exhibiting three prominent features: first, an unconventional magnetoresistance hysteresis that directly evidences time-reversal symmetry breaking and remains robust under different magnetic field orientations, fundamentally distinct from vortex pinning or long-range magnetic order; continuous oxygen reduction simultaneously weakens both superconductivity and the hysteresis, revealing their connection to specific Ni 3d electronic orbitals. Second, the current–voltage response demonstrates magnetic history dependence and non-reciprocity under zero field, further confirming spontaneous intrinsic time-reversal symmetry breaking. Third, the resistance exhibits slow logarithmic relaxation after removing the magnetic field, a hallmark of glassy dynamics. These phenomena reveal for the first time in nickel-based superconductors a superconducting state that simultaneously possesses spontaneous time-reversal symmetry breaking and intrinsic glassy characteristics, providing significant phenomenological and conceptual breakthroughs for understanding the mechanism of high-temperature superconductivity.
Materials
- (La,Pr,Sm)3Ni2O7
- La1.95Pr1.05Ni2O7
- La2.85Pr0.15Ni2O7
- La2.46Pr0.24Sm0.3Ni2O7
Methods
- electrical transport measurements
- magnetoresistance
- current-voltage (I-V) characteristics
- Hall effect
- Berezinskii-Kosterlitz-Thouless (BKT) analysis
- time-dependent resistance relaxations
- oxygen content modulation
Keywords
- time reversal symmetry breaking
- electronic glass
- superconducting glass state
- magnetoresistance hysteresis
- non reciprocal transport
- logarithmic resistance relaxation
- spin glass
- orbital selectivity
Highlights
- The unconventional magnetoresistance hysteresis is robust under different magnetic field orientations and differs fundamentally from trapped vortices or long-range-ordered magnetism.
- Successive oxygen reductions simultaneously weaken both the superconductivity and hysteresis, revealing their mutual connections to selective electronic orbitals.
- The non-reciprocal current-voltage response is magnetic field history-dependent, exhibiting highly effective field-tunability and memory effect.
- Logarithmically slow resistance relaxations upon removal of magnetic field are hallmarks of glassy dynamics.
Conclusions
- Through electrical transport study, we report the discovery of time-reversal symmetry breaking superconductivity with electronic glass in bilayer nickelate (La,Pr,Sm)3Ni2O7 films.
- It emerges in the lower-temperature regime of superconducting transition to the zero-resistance state, and is captured by three remarkable characteristics: unconventional magnetoresistance hysteresis, magnetic field history-dependence and zero-field non-reciprocity in current-voltage responses, and logarithmically slow resistance relaxations.
- Our findings uncover an unprecedented superconducting state in the nickelate superconductors, providing phenomenological and conceptual advances for future research on high-Tc superconductivity.
Main claims
- Unconventional magnetoresistance hysteresis provides direct evidence of time-reversal symmetry breaking, distinct from trapped vortices or long-range magnetism.
- Evidence: abstract: 'Unconventional magnetoresistance hysteresis, the direct evidence of TRS breaking',full_text: hysteresis observed under both out-of-plane and in-plane fields, with coalescing minima at zero field
- Magnetic field history-dependence and zero-field non-reciprocity in I-V responses substantiate intrinsic and spontaneous TRS breaking.
- Evidence: abstract: 'Magnetic field history-dependence and zero-field non-reciprocity',full_text Fig. 3a-f show clear deviation between V(I+) and |V(I-)| at zero field
- Logarithmically slow resistance relaxations after field removal are hallmarks of glassy dynamics.
- Evidence: abstract: 'Logarithmically slow resistance relaxations upon the removal of magnetic field, the hallmarks of glassy dynamics',full_text Fig. 5b-g show R_S(τ) ∝ -β log10 τ below 28K
- Successive oxygen reductions simultaneously weaken both superconductivity and hysteresis, revealing connection to selective electronic orbitals (likelyNi 3dx2-y2).
- Evidence: abstract: 'Successive oxygen reductions simultaneously weaken both the superconductivity and hysteresis',full_text Fig. 4a-d show systematic suppression with decreasing oxygen content
Workflow
- film_synthesis — High-quality single-crystalline films prepared.
- Materials: (La,Pr,Sm)3Ni2O7 thin films with various compositions
- Methods: gigantic-oxidative atomic-layer-by-layer epitaxy (GAE); on SrLaAlO4 (001) substrates
- Observations: RHEED oscillations confirm layer-by-layer growth; XRD confirms pure phase
- transport_measurements — Three key signatures of TRS breaking glass superconductivity observed.
- Materials: three compositions: La1.95Pr1.05Ni2O7, La2.85Pr0.15Ni2O7, La2.46Pr0.24Sm0.3Ni2O7
- Methods: four-electrode transport; magnetoresistance; Hall effect; current-voltage (I-V) characteristics
- Observations: BKT transition, T_c^onset ≈48 K, T_c^zero ≈17K; hysteretic magnetoresistance below 26K; non-reciprocal I-V; logarithmic resistance relaxation