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LaBollita, Harrison

Publications and source records attributed to LaBollita, Harrison.

8 records
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DOE OSTI2024

Assessing spin-density wave formation in La 3 Ni 2 O 7 from electronic structure calculations

Here, we employ correlated density-functional theory methods (DFT + Hubbard U) to investigate the spin-density wave state of the bilayer Ruddlesden-Popper (RP) nickelate La 3 Ni 2 O 7 which becomes superconducting under pressure. We predict that the ground state of this bilayer RP material has traits of both the double spin-stripe and the single spin-charge stripe phases proposed in the literature as it corresponds to in-plane up/up′/down/down′ diagonal stripes with up/down being high spin (formally Ni 2+ : d 8 ), and up′ /down′ being low spin (formally Ni 3+ : d 7 ). The main feature of this solution (that is insulating even at U = 0) is the dominant role of the d x 2 −y 2 bands around the Fermi level, which would become doped with the introduction of electrons via oxygen vacancies. In spite of the similarity with cuprates in terms of the dominant role of d x 2 −y 2 bands, some differences are apparent in the magnetic ground state of La 3 Ni 2 O 7 : the antiferromagnetic out-of-plane coupling within the bilayer (linked to the d z 2 orbitals forming a spin-singlet-like configuration) is found to be the dominant one while in-plane interactions are reduced due to the stripe order of the ground state. With pressure, this striped magnetic ground state remains similar in nature but the increase in bandwidth quickly transitions La 3 Ni 2 O 7 into a metallic state with all the activity close to the Fermi level involving, to a large extent, d x 2 −y 2 orbitals. This is reminiscent of the cuprates and may provide key insights into how superconductivity arises in this material under pressure.

LaBollita, Harrison↗
DOE OSTI2024

Electronic structure and magnetic tendencies of trilayer La 4 Ni 3 O 10 under pressure: Structural transition, molecular orbitals, and layer differentiation

Motivated by the recent observation of superconductivity in the pressurized trilayer Ruddlesden-Popper (RP) nickelate La 4 Ni 3 O 10 , we explore its structural, electronic, and magnetic properties as a function of hydrostatic pressure from first-principles calculations. We find that an orthorhombic (monoclinic)-to-tetragonal transition under pressure takes place concomitantly with the onset of superconductivity. The electronic structure of La 4 Ni 3 O 10 can be understood using a molecular trimer basis wherein n molecular subbands arise as the d z 2 orbitals hybridize strongly along the c axis within the trilayer. The magnetic tendencies indicate that the ground state at ambient pressure is formed by nonmagnetic inner planes and stripe-ordered outer planes that are antiferromagnetically coupled along the c axis, resulting in an unusual ↑, 0, ↓ stacking that is consistent with the spin density wave model previously suggested by neutron diffraction. Such a state is destabilized at the pressure where superconductivity arises. Despite the presence of d z 2 states at the Fermi level, the d x 2 –y 2 orbitals also play a key role in the electronic structure of La4Ni3O10. Finally, this active role of the d x 2 –y 2 states in the low-energy physics of the trilayer RP nickelate, together with the distinct electronic behavior of the inner and outer planes, resembles the physics of multilayer cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Polymorphism in the Ruddlesden–Popper Nickelate La 3 Ni 2 O 7 : Discovery of a Hidden Phase with Distinctive Layer Stacking

We report the discovery of a novel form of Ruddlesden–Popper (RP) nickelate that stands as the first example of long-range, coherent polymorphism in this class of inorganic solids. Rather than the well-known, uniform stacking of perovskite blocks ubiquitously found in RP phases, this newly discovered polymorph of the bilayer RP phase La 3 Ni 2 O 7 adopts a novel stacking sequence in which single-layer and trilayer blocks of NiO 6 octahedra alternate in a “1313” sequence. Crystals of this new polymorph are described in space group Cmmm, although we note evidence for a competing Imam variant. Transport measurements at ambient pressure reveal metallic character with evidence of a charge density wave transition with an onset at T ≈ 134 K. In conclusion, the discovery of such polymorphism could reverberate to the expansive range of science and applications that rely on RP materials, particularly the recently reported signatures of superconductivity in bilayer La 3 Ni 2 O 7 with T c as high as 80 K above 14 GPa.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Limits to the strain engineering of layered square-planar nickelate thin films

The layered square-planar nickelates, Nd n+1 Ni n O 2n+2 , are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd 6 Ni 5 O 12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n = 3 Ruddlesden-Popper compound, Nd 4 Ni 3 O 10 , and subsequent reduction to the square-planar phase, Nd 4 Ni 3 O 8 . We synthesize our highest quality Nd 4 Ni 3 O 10 films under compressive strain on LaAlO 3 (001), while Nd 4 Ni 3 O 10 on NdGaO 3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd 4 Ni 3 O 10 on SrTiO 3 (001). Films reduced on LaAlO 3 become insulating and form compressive strain-induced c-axis canting defects, while Nd 4 Ni 3 O 8 films on NdGaO 3 are metallic. This work provides a pathway to the synthesis of Nd n+1 Ni n O 2n+2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Antiferromagnetic metal phase in an electron-doped rare-earth nickelate

Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in non-collinear or non-centrosymmetric spin structures. The rare-earth nickelate NdNiO 3 is known to be a non-collinear antiferromagnet in which the onset of antiferromagnetic ordering is concomitant with a transition to an insulating state. In this work, we find that for low electron doping, the magnetic order on the nickel site is preserved, whereas electronically, a new metallic phase is induced. We show that this metallic phase has a Fermi surface that is mostly gapped by an electronic reconstruction driven by bond disproportionation. Furthermore, we demonstrate the ability to write to and read from the spin structure via a large zero-field planar Hall effect. Our results expand the already rich phase diagram of rare-earth nickelates and may enable spintronics applications in this family of correlated oxides.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Visualizing the out-of-plane electronic dispersions in an intercalated transition metal dichalcogenide

Layered transition metal dichalcogenides have a rich phase diagram and they feature two-dimensionality in numerous physical properties. Co 1/3 NbS 2 is one of the newest members of this family where Co atoms are intercalated into the van der Waals gaps between NbS 2 layers. Here, we study the three-dimensional electronic band structure of Co 1/3 NbS 2 using both surface and bulk sensitive angle-resolved photoemission spectroscopy. We show that the electronic bands do not fit into the rigid band shift picture after the Co intercalation. Instead, Co 1/3 NbS 2 displays a different orbital character near the Fermi level compared to the pristine NbS 2 compound and has a clear band dispersion in the k z direction despite its layered structure. Our photoemission study demonstrates the out-of-plane electronic correlations introduced by the Co intercalation, thus offering a different perspective on this compound. Finally, we propose how Fermi level tuning could lead to exotic phases such as spin density wave instability.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Superconductivity in a quintuple-layer square-planar nickelate

Since the discovery of high-temperature superconductivity in the copper oxide materials, there have been sustained efforts to both understand the origins of this phase and discover new cuprate-like superconducting materials. One prime materials platform has been the rare-earth nickelates and indeed superconductivity was recently discovered in the doped compound Nd 0.8 Sr 0.2 NiO 2 . Undoped NdNiO 2 belongs to a series of layered square-planar nickelates with chemical formula Nd n+1 Ni n O 2n+2 and is known as the 'infinite-layer' (n=∞) nickelate. Furthermore, we report the synthesis of the quintuple-layer (n=5) member of this series, Nd 6 Ni 5 O 12 , in which optimal cuprate-like electron filling (d 8.8 ) is achieved without chemical doping. We observe a superconducting transition beginning at ~13 K. Electronic structure calculations, in tandem with magnetoresistive and spectroscopic measurements, suggest that Nd 6 Ni 5 O 12 interpolates between cuprate-like and infinite-layer nickelate-like behavior. In engineering a distinct superconducting nickelate, we identify the square-planar nickelates as a new family of superconductors which can be tuned via both doping and dimensionality.

36 MATERIALS SCIENCE↗