Oxygen deficiency is known to critically influence the superconductivity of La3Ni2O7-δ.However,precise control of oxygen content to mitigate such deficiencies remains a significant challenge.In this work,we ...Oxygen deficiency is known to critically influence the superconductivity of La3Ni2O7-δ.However,precise control of oxygen content to mitigate such deficiencies remains a significant challenge.In this work,we synthesized high-oxygencontent La3Ni2O7+δpolycrystals via high-pressure oxygen annealing with the oxygen stoichiometry(δ)successfully tuned by varying the amount of KClO4.The obtained samples La3Ni2O7.16and La3Ni2O7.38exhibit metallic behavior at ambient pressure.We further conducted a comprehensive investigation into the pressure-induced superconductivity and atomic structure.STEM imaging revealed large-area bilayer-phase stacking in La3Ni2O7.16,while La3Ni2O7.38showed noticeable intergrowth with other Ruddlesden-Popper(R-P)phases.Notably,the critical pressure in La3Ni2O7.16is substantially reduced,though its critical temperature(Tc)is lower than that of as-grown samples.In contrast,only a weak superconducting signal was detected in higher oxygen content sample La3Ni2O7.38likely due to the intergrowth with other R-P phases,nonnegligible interstitial oxygen,or an increased fraction of the tetragonal phase.Our findings provide a viable pathway for optimizing nickelate superconductivity and offer insights into the fundamental mechanisms governing superconductivity in these materials.展开更多
基金Project supported by the National Key R&D Program of China(Grant No.2022YFA1403203)the National Natural Science Foundation of China(Grant Nos.12204007,12374133,12304162,and 12074002)+5 种基金the Key Scientific Research Foundation of the Education Department of Anhui Province(Grant No.2024AH050046)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302802)Quantum Science and TechnologyNational Science and Technology Major Project(Grant No.2024ZD0301300)the Major Basic Program of Natural Science Foundation of Shandong Province(Grant No.ZR2021ZD01)the Start-up Funding Program of Guangdong-Hong Kong-Macao Greater Bay Area Quantum Science Center(Grant No.QD2301003)Guangdong Provincial Quantum Science Strategic Initiative(Grant No.GDZX2401001)。
摘要Oxygen deficiency is known to critically influence the superconductivity of La3Ni2O7-δ.However,precise control of oxygen content to mitigate such deficiencies remains a significant challenge.In this work,we synthesized high-oxygencontent La3Ni2O7+δpolycrystals via high-pressure oxygen annealing with the oxygen stoichiometry(δ)successfully tuned by varying the amount of KClO4.The obtained samples La3Ni2O7.16and La3Ni2O7.38exhibit metallic behavior at ambient pressure.We further conducted a comprehensive investigation into the pressure-induced superconductivity and atomic structure.STEM imaging revealed large-area bilayer-phase stacking in La3Ni2O7.16,while La3Ni2O7.38showed noticeable intergrowth with other Ruddlesden-Popper(R-P)phases.Notably,the critical pressure in La3Ni2O7.16is substantially reduced,though its critical temperature(Tc)is lower than that of as-grown samples.In contrast,only a weak superconducting signal was detected in higher oxygen content sample La3Ni2O7.38likely due to the intergrowth with other R-P phases,nonnegligible interstitial oxygen,or an increased fraction of the tetragonal phase.Our findings provide a viable pathway for optimizing nickelate superconductivity and offer insights into the fundamental mechanisms governing superconductivity in these materials.