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arXiv 2408.09421cond-mat.str-elcond-mat.supr-con
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化学压力与物理压力对双层镍酸盐结构转变的影响

Chemical versus physical pressure effects on the structure transition of bilayer nickelates

Gang Wang, Ningning Wang, Tenglong Lu, Stuart Calder, Jiaqiang Yan, Lifen Shi, Jun Hou, Liang Ma, Lili Zhang, Jianping Sun, Bosen Wang, Sheng Meng, Miao Liu, Jinguang Cheng

AI总结:

本研究结合实验与理论,发现化学压力(小半径稀土离子替换La³⁺)会增大双层镍酸盐的正交畸变、提升结构转变临界压力,提出用大半径阳离子部分取代La³⁺或是实现常压高Tc超导的可行方向。

摘要:

双层La₃Ni₂O₇中高压诱导的正交-四方结构转变伴随高Tc超导(HTSC)的发现,点燃了通过在常压下稳定四方相实现高Tc超导的希望。为模拟外部物理压力的效应,通过用更小的稀土R³⁺替换La³⁺施加化学压力被认为是一种潜在途径。本研究通过实验与理论相结合的研究,阐明了化学压力和物理压力对双层镍酸盐结构转变的不同作用。与普遍预期相反,我们发现在La₃₋ₓRₓNi₂O₇₋δ中用更小的R³⁺取代La³⁺,尽管整体晶格发生收缩,却会产生更强的正交结构畸变,因此需要更高的压力才能诱导结构转变。我们建立了结构转变的临界压力Pc与A位阳离子平均尺寸之间的定量关系。对Pc与<r_A>(A位阳离子平均半径)进行线性外推,得到在Pc约为1 bar时,推定的临界<r_A>_c值约为1.23埃。Pc与<r_A>之间的负相关关系表明,通过用更小的R³⁺离子替换La³⁺不太可能将Pc降至常压。相反,用碱土金属Sr²⁺或Ba²⁺等更大的阳离子部分取代La³⁺可能是一种可行的方法。我们的研究结果为在双层镍酸盐中探索常压高Tc超导提供了有价值的指导。

英文摘要:

The observation of high-$T_c$ superconductivity (HTSC) in concomitant with pressure-induced orthorhombic-tetragonal structural transition in the bilayer La$_{3}$Ni$_2$O$_7$ has sparked hopes of achieving HTSC by stabilizing the tetragonal phase at ambient pressure. To mimic the effect of external physical pressures, the application of chemical pressure via replacing La$^3$$^+$ with smaller rare-earth R$^3$$^+$ has been considered as a potential route. Here we clarify the distinct effects of chemical and physical pressures on the structural transition of bilayer nickelates through a combined experimental and theoretical investigation. Contrary to general expectations, we find that substitutions of smaller R$^3$$^+$ for La$^3$$^+$ in La$_{3-x}$R$_x$Ni$_2$O$_{7-δ}$, despite of an overall lattice contraction, produce stronger orthorhombic structural distortions and thus require higher pressures to induce the structural transition. We established a quantitative relationship between the critical pressure $P_c$ for structural transition and the average size of $A$-site cations. A linear extrapolation of $P_c$ versus <$r_A$> yields a putative critical value of <$r_A$>$_c$ ~ 1.23 angstrom for $P_c$ ~ 1 bar. The negative correlation between $P_c$ and <$r_A$> indicates that it is unlikely to reduce $P_c$ to ambient by replacing La$^3$$^+$ with smaller R$^3$$^+$ ions. Instead, partial substitution of La$^3$$^+$ with larger cations such as alkaline-earth Sr$^2$$^+$ or Ba$^2$$^+$ might be a feasible approach. Our results provide valuable guidelines in the quest of ambient-pressure HTSC in bilayer nickelates.

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