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Phase Diagram of Infinite Layer Praseodymium Nickelate Pr$_{1-x}$Sr$_{x}$NiO$_2$ Thin Films

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 Added by Motoki Osada
 Publication date 2020
  fields Physics
and research's language is English




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We report the phase diagram of infinite layer Pr$_{1-x}$Sr$_{x}$NiO$_2$ thin films synthesized via topotactic reduction from the perovskite precursor phase using CaH$_2$. Based on the electrical transport properties, we find a doping-dependent superconducting dome extending between $x$ = 0.12 and 0.28, with a maximum superconducting transition temperature $T_{rm{c}}$ of 14 K at $x$ = 0.18, bounded by weakly insulating behavior on both sides. In contrast to the narrower dome observed in Nd$_{1-x}$Sr$_{x}$NiO$_2$, a local $T_{rm{c}}$ suppression near $x$ = 0.2 was not observed for the Pr$_{1-x}$Sr$_{x}$NiO$_2$ system. Normal state Hall effect measurements indicate mixed carrier contributions of both electrons and holes, and show a sign change in the Hall coefficient as functions of temperature and $x$, quite similar to that in Nd$_{1-x}$Sr$_{x}$NiO$_2$. Also similar is the observation of a minimum in the normal state resistivity associated with the superconducting compositions. These findings indicate an infinite layer nickelate phase diagram that is relatively insensitive to the rare-earth element, but suggest that disorder arising from the variations of the ionic radii on the rare-earth site affects the superconducting dome.



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To understand the superconductivity recently discovered in Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, we carried out LDA+DMFT (local density approximation plus dynamical mean-field theory) and magnetic force response calculations. The on-site correlation in Ni-$3d$ orbitals causes notable changes in the electronic structure. The calculated temperature-dependent susceptibility exhibits the Curie-Weiss behavior, indicating the localized character of its moment. From the low-frequency behavior of self-energy, we conclude that the undoped phase of this nickelate is Fermi-liquid-like contrary to cuprates. Interestingly, the estimated correlation strength by means of the inverse of quasiparticle weight is found to increase and then decrease as a function of hole concentration, forming a dome-like shape. Another finding is that magnetic interactions in this material become two-dimensional by hole doping. While the undoped NdNiO$_2$ has the sizable out-of-plane interaction, hole dopings strongly suppress it. This two-dimensionality is maximized at the hole concentration $deltaapprox0.25$. Further analysis as well as the implications of our findings are presented.
The recent observation of superconductivity in infinite-layer nickelate Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$ has received considerable attention. Despite the many efforts to understand the superconductivity in infinite-layer nickelates, a consensus on the underlying mechanism for the superconductivity has yet to be reached, partly owing to the challenges with the material synthesis. Here, we report the successful growth of superconducting infinite-layer Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$ films by pulsed-laser deposition and soft chemical reduction. The details on growth process will be discussed.
A variety of nickel oxide compounds have long been studied for their manifestation of various correlated electron phenomena. Recently, superconductivity was observed in nanoscale infinite layer nickelate thin films of Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, epitaxially stabilized on SrTiO$_3$ substrates via topotactic reduction from the perovskite precursor phase. Here we present the synthesis and properties of PrNiO$_2$ thin films on SrTiO$_3$. Upon doping in Pr$_{0.8}$Sr$_{0.2}$NiO$_2$, we observe superconductivity with a transition temperature of 7-12 K, and robust critical current density at 2 K of 334 kA/cm$^2$. These findings indicate that superconductivity in the infinite layer nickelates is relatively insensitive to the details of the rare earth 4$f$ configuration. Furthermore, they motivate the exploration of a broader family of compounds based on two-dimensional NiO$_2$ planes, which will enable systematic investigation of the superconducting and normal state properties and their underlying mechanisms.
The recent discovery of superconductivity in infinite-layer nickelates has motivated tremendous efforts to study these materials that are analogous to cuprates. However, superconductivity in infinite-layer nickelates has been realized only in thin films grown on SrTiO$_3$ substrates, thus raising the question whether it is interface-induced and the query into the role of SrTiO$_3$ substrate. Here, we report the observation of superconductivity in Pr$_{0.8}$Sr$_{0.2}$NiO$_2$ films prepared at almost the same conditions except they are grown on different substrates (LaAlO$_3$)$_{0.3}$(Sr$_2$AlTaO$_6$)$_{0.7}$ (LSAT) and SrTiO$_3$ with the corresponding onset of superconductivity maximized at 15 K and 9K, respectively. Our results not only suggest that the superconductivity in infinite-layer nickelates is unlikely an interface-induced phenomenon and that the SrTiO$_3$ substrate is not a necessary for the emergence of superconductivity, but also indicate that the compressive strain can possibly increase T$_c$ of Pr$_{0.8}$Sr$_{0.2}$NiO$_2$.
Infinite-layer Nd1-xSrxNiO2 thin films with Sr doping level x from 0.08 to 0.3 were synthesized and investigated. We found a superconducting dome to be between 0.12 and 0.235 which is accompanied by a weakly insulating behaviour in both underdoped and overdoped regimes. The dome is akin to that in the electron-doped 214-type and infinite-layer cuprate superconductors. For x higher than 0.18, the normal state Hall coefficient ($R_{H}$) changes the sign from negative to positive as the temperature decreases. The temperature of the sign changes monotonically decreases with decreasing x from the overdoped side and approaches the superconducting dome at the mid-point, suggesting a reconstruction of the Fermi surface as the dopant concentration changes across the center of the dome.
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