DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Bulk high-temperature superconductivity in pressurized tetragonal La2PrNi2O7

Journal Article · · Nature (London)
ORCiD logo [1];  [1];  [2];  [1]; ORCiD logo [1];  [3];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [4];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1] more »; ORCiD logo [1]; ORCiD logo [5];  [6];  [6]; ORCiD logo [7]; ORCiD logo [7]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [6]; ORCiD logo [1] « less
  1. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS); University of Chinese Academy of Sciences, Beijing (China)
  2. Univ. of Tokyo (Japan); Shanghai Jiao Tong Univ. (China)
  3. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS)
  4. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS); Univ. of Tokyo (Japan)
  5. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS); University of Chinese Academy of Sciences, Beijing (China); New Cornerstone Science Laboratory, Beijing (China)
  6. Univ. of Tokyo (Japan)
  7. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

The Ruddlesden–Popper (R–P) bilayer nickelate, La3Ni2O7, was recently found to show signatures of high-temperature superconductivity (HTSC) at pressures above 14 GPa . Subsequent investigations achieved zero resistance in single-crystalline and polycrystalline samples under hydrostatic pressure conditions. Yet, obviousdiamagnetic signals, the other hallmark of superconductors, are still lacking owing to the flamentary nature with low superconducting volume fraction. The presence of a new 1313 polymorph and competing R–P phases obscured proper identification of the phase for HTSC. Thus, achieving bulk HTSC and identifying the phase at play are the most prominent tasks. Here we address these issues in the praseodymium (Pr)-doped La2PrNi2O7 polycrystalline samples. We find that substitutions of Pr for La efectively inhibit the intergrowth of diferent R–P phases, resulting in a nearly pure bilayer structure. For La2PrNi2O7, pressure-induced orthorhombic to tetragonalstructural transition takes place at Pc ≈ 11 GPa, above which HTSC emerges gradually on further compression. The superconducting transition temperatures at 18–20 GPa reach $$T$$ $$^{onset}_{c}$$ = $82.5$ $$K$$ and $$T$$ $$^{zero}_{c}$$ = $60$ $$K$$, which are the highest values, to our knowledge, among known nickelate superconductors. Importantly, bulk HTSC was testified by detecting clear diamagnetic signals below about 75 K with appreciable superconducting shielding volume fractions at a pressure of above 15 GPa. Further, our results not only resolve the existing controversies but also provide directions for exploring bulk HTSC in the bilayer nickelates.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2481168
Journal Information:
Nature (London), Journal Name: Nature (London) Journal Issue: 8034 Vol. 634; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (39)

Synthesis, Structure, and Properties of the Layered Perovskite La3Ni2O7-δ journal February 1994
Synthesis, Structure, and Properties of Ln4Ni3O10-δ (Ln = La, Pr, and Nd) journal July 1995
Evidence for charge and spin density waves in single crystals of La3Ni2O7 and La3Ni2O6 journal November 2022
Magnetic properties of quasi-two-dimensional La2NiO4 journal October 1986
Long-Range Structural Order in a Hidden Phase of Ruddlesden–Popper Bilayer Nickelate La3Ni2O7 journal March 2024
Electro-Oxidation Reaction of Methanol over La2–xSrxNiO4+δ Ruddlesden–Popper Oxides journal January 2022
Structure Responsible for the Superconducting State in La3Ni2O7 at High-Pressure and Low-Temperature Conditions journal March 2024
Polymorphism in the Ruddlesden–Popper Nickelate La3Ni2O7: Discovery of a Hidden Phase with Distinctive Layer Stacking journal January 2024
Crystal and Electronic Structure of FeSe at High Pressure and Low Temperature journal October 2010
Dome-shaped magnetic order competing with high-temperature superconductivity at high pressures in FeSe journal July 2016
Structural phase transition, s±-wave pairing, and magnetic stripe order in bilayered superconductor La3Ni2O7 under pressure journal March 2024
Orbital-dependent electron correlation in double-layer nickelate La3Ni2O7 journal May 2024
Electronic correlations and partial gap in the bilayer nickelate La3Ni2O7 journal August 2024
Electronic and magnetic excitations in La3Ni2O7 journal November 2024
Optical properties and electronic correlations in La3Ni2O7 bilayer nickelates under high pressure journal November 2024
High-temperature superconductivity with zero resistance and strange-metal behaviour in La3Ni2O7−δ journal June 2024
Signatures of superconductivity near 80 K in a nickelate under high pressure journal July 2023
Visualization of oxygen vacancies and self-doped ligand holes in La3Ni2O7−δ journal June 2024
Integrated-fin gasket for palm cubic-anvil high pressure apparatus journal September 2014
Emergence of High-Temperature Superconducting Phase in Pressurized La3Ni2O7 Crystals journal October 2023
Type-II t−J model and shared superexchange coupling from Hund's rule in superconducting La3Ni2O7 journal November 2023
Absence of Ni2+/Ni3+ charge disproportionation and possible roles of O 2⁢𝑝 holes in La3⁢Ni2⁢O7−𝛿 revealed by hard x-ray photoemission spectroscopy journal March 2024
Influence of oxygen stoichiometry on the antiferromagnetic ordering of single crystals ofLa2NiO4+δ journal January 1992
High- T c Superconductivity in FeSe at High Pressure: Dominant Hole Carriers and Enhanced Spin Fluctuations journal April 2017
Bilayer Two-Orbital Model of La3Ni2O7 under Pressure journal September 2023
Correlated Electronic Structure of La3Ni2O7 under Pressure journal November 2023
s± -Wave Pairing and the Destructive Role of Apical-Oxygen Deficiencies in La3Ni2O7 under Pressure journal December 2023
Bilayer t−J−J⊥ Model and Magnetically Mediated Pairing in the Pressurized Nickelate La3Ni2O7 journal January 2024
Possible High Tc Superconductivity in La3Ni2O7 under High Pressure through Manifestation of a Nearly Half-Filled Bilayer Hubbard Model journal March 2024
Pressure Driven Fractionalization of Ionic Spins Results in Cupratelike High- Tc Superconductivity in La3Ni2O7 journal March 2024
Interlayer-Coupling-Driven High-Temperature Superconductivity in La3Ni2O7 under Pressure journal April 2024
High oxygen pressure floating zone growth and crystal structure of the metallic nickelates R 4 Ni 3 O 10 ( R = La , Pr ) journal August 2020
Design and synthesis of three-dimensional hybrid Ruddlesden-Popper nickelate single crystals journal May 2024
GSAS-II : the genesis of a modern open-source all purpose crystallography software package journal March 2013
139La NQR Study of Antiferromagnetic La2NiO4+δ journal August 1989
Studies on Successive Electronic State Changes in Systems with NiO2Planes –139La-NMR/NQR– journal September 2001
Simultaneous measurement of pressure evolution of crystal structure and superconductivity in FeSe 0.92 using designer diamonds journal July 2012
Electronic structure and superconductivity in bilayer La3Ni2O7 preprint February 2024
Multiband Metallic Ground State in Multilayered Nickelates La3Ni2O7 and La4Ni3O10 Probed by 139La-NMR at Ambient Pressure journal May 2024