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Register a new userFundamental difference in the electronic reconstruction of infinite-layer vs. perovskite neodymium nickelate films on SrTiO$_3$(001)
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Motivated by recent reports of superconductivity in Sr-doped NdNiO$_2$ films on SrTiO$_3$(001) [Nature (London) 572, 624 (2019)], we explore the role of the polar interface on the structural and electronic properties of NdNiO$_n$/SrTiO$_3$(001) ($n=2,3$) by performing first-principles calculations including a Coulomb repulsion term. For infinite-layer nickelate films ($n=2$), electronic reconstruction drives the surprising emergence of a two-dimensional electron gas (2DEG) at the interface involving a strong occupation of the Ti $3d$ states. This effect is more pronounced than in LaAlO$_3$/SrTiO$_3$(001) and accompanied by a substantial reconstruction of the Fermi surface: a depletion of the self-doping Nd $5d$ states and an enhanced Ni $e_g$ orbital polarization reaching up to $35%$ at the surface, reflecting a single hole in the $3d_{x^2-y^2}$ states, i.e., cuprate-like behavior. In contrast, no 2DEG forms for perovskite films ($n=3$) or if a single perovskite layer persists at the interface. We show that the topotactic reaction from the perovskite to the infinite-layer phase is confined to the nickelate film, whereas the SrTiO$_3$ substrate remains intact.
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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.
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.
Scanning tunneling microscopy and spectroscopy are utilized to study the atomic-scale structure and electronic properties of infinite-layer Sr0.94La0.06CuO2+y films prepared on SrRuO3-buffered SrTiO3(001) substrate by ozone-assisted molecular beam epitaxy. Incommensurate structural supermodulation with a period of 24.5{AA} is identified on the CuO2-terminated surface, leading to characteristic stripes running along the 45o direction with respect to the Cu-O-Cu bonds. Spatially resolved tunneling spectra reveal substantial inhomogeneity on a nanometer length scale and emergence of in-gap states at sufficient doping. Despite the Fermi level shifting up to 0.7 eV, the charge-transfer energy gap of the CuO2 planes remains fundamentally unchanged at different doping levels. The occurrence of the CuO2 superstructure is constrained in the surface region and its formation is found to link with oxygen intake that serves as doping agent of holes in the epitaxial films.
Hole-doped perovskite bismuthates such as Ba$_{1-x}$K$_x$BiO$_3$ and Sr$_{1-x}$K$_x$BiO$_3$ are well-known bismuth-based oxide high-transition-temperature superconductors. Reported thin bismuthate films show relatively low quality, likely due to their large lattice mismatch with the substrate and a low sticking coefficient of Bi at high temperatures. Here, we report the successful epitaxial thin film growth of the parent compound strontium bismuthate SrBiO$_3$ on SrO-terminated SrTiO$_3$ (001) substrates by molecular beam epitaxy. Two different growth methods, high-temperature co-deposition or recrystallization cycles of low-temperature deposition plus high-temperature annealing, are developed to improve the epitaxial growth. SrBiO$_3$ has a pseudocubic lattice constant $sim$4.25 AA, an $sim$8.8% lattice mismatch on SrTiO$_3$ substrate, leading to a large strain in the first few unit cells. Films thicker than 6 unit cells prepared by both methods are fully relaxed to bulk lattice constant and have similar quality. Compared to high-temperature co-deposition, the recrystallization method can produce higher quality 1-6 unit cell films that are coherently or partially strained. Photoemission experiments reveal the bonding and antibonding states close to the Fermi level due to Bi and O hybridization, in good agreement with density functional theory calculations. This work provides general guidance to the synthesis of high-quality perovskite bismuthate films.
SrTiO$_3$ is an incipient ferroelectric on the verge of a polar instability, which is avoided at low temperatures by quantum fluctuations. Within this unusual quantum paraelectric phase, superconductivity persists despite extremely dilute carrier densities. Ferroelectric fluctuations have been suspected to play a role in the origin of superconductivity by contributing to electron pairing. To investigate this possibility, we used optical second harmonic generation to measure the doping and temperature dependence of the ferroelectric order parameter in compressively strained SrTiO$_3$ thin films. At low temperatures, we uncover a spontaneous out-of-plane ferroelectric polarization with an onset that correlates perfectly with normal-state electrical resistivity anomalies. These anomalies have previously been associated with an enhancement of the superconducting critical temperature in doped SrTiO$_3$ films, directly linking the ferroelectric and superconducting phases. We develop a long-range mean-field Ising model of the ferroelectric phase transition to interpret the data and extract the relevant energy scales in the system. Our results support a long-suspected connection between ferroelectricity and superconductivity in SrTiO$_3$, but call into question the role played by ferroelectric fluctuations.
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