摘要
本研究通过系统调控La3Ni2O7+δ系列样品的氧含量,合成了不同相组成的材料,包括纯双层相、双层与单层-双层杂化相混合相以及含三层交生的主双层相。高压输运测量表明,这些相分别对应不同的超导转变温度(T_c),其中双层相呈现约80 K的超导电性,杂化相和三层交生相的T_c较低。氧含量不仅影响相纯度,还直接调控双层超导电性的上临界场(H_c2),纯双层相具有更高的H_c2。通过建立T_c和H_c2随氧含量变化的相图,本研究实现了对Ruddlesden-Popper镍酸盐氧含量的精确控制,为理解其高压超导机制提供了关键实验依据。
材料
方法
- high-pressure transport
- X-ray diffraction
- compositional analysis
关键词
- oxygen content
- phase purity
- upper critical field
- intergrowth phases
- bilayer phase
亮点
- Establishes a phase diagram of Tc and Hc2 as functions of oxygen content in La3Ni2O7+δ.
结论
- Oxygen content governs phase purity, controlling the presence of hybrid phases and trilayer intergrowths.
- Superconducting transitions with contrasting Tc values correspond to different phase fractions.
- The upper critical field (Hc2) of the bilayer phase is directly modulated by oxygen content.
主要论断
- Oxygen content in La3Ni2O7+δ controls the formation of intergrowth phases: low oxygen promotes hybrid-1212, high oxygen promotes trilayer inclusions.
- 证据: NPD and STEM show hybrid-1212 phase in oxygen-deficient sample (δ=-0.14); trilayer intergrowths in oxygen-rich samples (δ>0)
- Different RP phases show distinct superconducting transition temperatures: bilayer ≈80 K, hybrid-1212 ≈70 K, trilayer ≈4-6 K.
- 证据: High-pressure transport at 25.5 GPa shows multiple transitions with these T_c values
- The upper critical field H_c2 of the bilayer superconductivity is strongly modulated by oxygen content, peaking near stoichiometric composition.
- 证据: Ginzburg-Landau fitting of transport under field shows that H_c2 increases with oxygen content up to δ=0, then decreases for higher δ
研究流程
- sample_synthesis — Systematic control of oxygen content in La3Ni2O7+δ.
- 材料: La2O3; NiO; Ni(NO3)2·6H2O
- 方法: solid-state reaction; sol-gel method; controlled annealing in H2/N2, O2, and high-pressure O2
- 观察: six samples with oxygen content δ from -0.34 to 0.08
- structural_and_compositional_analysis — Oxygen content governs NiO6 tilting and formation of intergrowth phases.
- 材料: polycrystalline La3Ni2O7+δ
- 方法: XAFS; NPD; SXRD; STEM; TGA
- 观察: oxygen content correlates with Ni valence and octahedral distortion; intergrowth phases identified
- high_pressure_electronic_transport — Different RP phases exhibit distinct T_c values under pressure.
- 材料: polycrystalline samples in DAC
- 方法: four-probe resistivity measurement under pressure with KBr pressure medium
- 观察: superconducting transitions with onset T_c ≈80 K for bilayer, ≈70 K for hybrid-1212, ≈5 K for trilayer
- upper_critical_field_analysis — Oxygen content directly modulates H_c2 of bilayer superconductivity.
- 材料: transport data at 25.5 GPa
- 方法: Ginzburg-Landau fitting
- 观察: H_c2 is modulated by oxygen content, peaking near stoichiometric composition