Engineering topics

Maier, Thomas A.

Publications and source records attributed to Maier, Thomas A..

At least 19 records

DOE OSTI2024

Magnetic phase diagram of a two-orbital model for bilayer nickelates with varying doping

Motivated by the recently discovered high-T c bilayer nickelate superconductor La 3⁢ Ni 2 ⁢O 7 , we comprehensively research a bilayer 2×2×2 cluster for different electronic densities n by using the Lanczos method. We also employ the random-phase approximation to quantify the first magnetic instability with increasing Hubbard coupling strength, also varying n. Based on the spin structure factor S(q), we have obtained a rich magnetic phase diagram in the plane defined by n and U/W, at fixed Hund coupling, where U is the Hubbard strength and W the bandwidth. We have observed numerous states, such as A-AFM, Stripes, G-AFM, and C-AFM. At half-filling, n=2 (two electrons per Ni site, corresponding to N=16 electrons), the canonical superexchange interaction leads to a robust G-AFM state (π,π,π) with antiferromagnetic couplings both in-plane and between layers. By increasing or decreasing electronic densities, ferromagnetic tendencies emerge from the “half-empty” and “half-full” mechanisms, leading to many other interesting magnetic tendencies. In addition, the spin-spin correlations become weaker both in the hole or electron doping regions compared with half-filling. At n=1.5 (or N=12), density corresponding to La 3 ⁢Ni 2 ⁢O 7 , we obtained the “Stripe 2” ground state (antiferromagnetic coupling in one in-plane direction, ferromagnetic coupling in the other, and antiferromagnetic coupling along the z axis) in the 2×2×2 cluster. In addition, we obtained a much stronger AFM coupling along the z axis than the magnetic coupling in the xy plane. The random-phase approximation calculations with varying n give very similar results as Lanczos, even though both techniques are based on quite different procedures. Additionally, a state with q/π=(0.6,0.6,1) close to the E-phase wavevector is found in our RPA calculations by slightly reducing the filling to n=1.25, possibly responsible for the E-phase SDW recently observed in experiments. In conclusion, our predictions can be tested by chemically doping La 3 ⁢Ni 2 ⁢O 7 .

36 MATERIALS SCIENCE↗

DOE OSTI2024

SmoQyDEAC.jl: A differential evolution package for the analytic continuation of imaginary time correlation functions

We introduce the SmoQyDEAC.jl package, a Julia implementation of the Differential Evolution Analytic Continuation (DEAC) algorithm [N. S. Nichols et al., Phys. Rev. E 106, 025312 (2022)] for analytically continuing noisy imaginary time correlation functions to the real frequency axis. Our implementation supports fermionic and bosonic correlation functions on either the imaginary time or Matsubara frequency axes, and treatment of the covariance error in the input data. This paper presents an overview of the DEAC algorithm and the features implemented in the SmoQyDEAC.jl package. It also provides detailed benchmarks of the package's output against the popular maximum entropy and stochastic analytic continuation methods.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2024

Prediction of s ± -Wave Superconductivity Enhanced by Electronic Doping in Trilayer Nickelates La 4 Ni 3 O 10 under Pressure

Motivated by the recently reported signatures of superconductivity in trilayer La 4 ⁢Ni 3 ⁢O 10 under pressure, here we comprehensively study this system using ab initio and random-phase approximation techniques. Without electronic interactions, the Ni d 3z 2 –r 2 orbitals show a bonding-antibonding and nonbonding splitting behavior via the O p z orbitals inducing a “trimer” lattice in La 4⁢ Ni 3 ⁢O 10 , analogous to the dimers of La 3 ⁢Ni 2 ⁢O 7 . The Fermi surface consists of three electron sheets with mixed e g orbitals, and a hole and an electron pocket made up of the d 3⁢z 2 –r 2 orbital, suggesting a Ni two-orbital minimum model. In addition, we find that superconducting pairing is induced in the s ± -wave channel due to partial nesting between the M = (π,π) centered pockets and portions of the Fermi surface centered at the Γ = (0,0) point. With changing electronic density n, the s ± instability remains leading and its pairing strength shows a domelike behavior with a maximum around n = 4.2 ( ~6.7% electron doping). The superconducting instability disappears at the same electronic density as that in the new 1313 stacking La 3 ⁢Ni 2 ⁢O 7 , correlated with the vanishing of the hole pocket that arises from the trilayer sublattice, suggesting that the high-T c superconductivity of La 3⁢ Ni 2 ⁢O 7 does not originate from a trilayer and monolayer structure. Furthermore, we confirm the experimentally proposed spin state in La 4 ⁢Ni 3 ⁢O 10 with an in-plane (π, π) order and antiferromagnetic coupling between the top and bottom Ni layers, and spin zero in the middle layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Electronic structure, self-doping, and superconducting instability in the alternating single-layer trilayer stacking nickelates La 3 ⁢Ni 2 ⁢O 7

Motivated by the recently proposed alternating single-layer trilayer stacking structure for the nickelate La 3 ⁢Ni 2 ⁢O 7 , we comprehensively study this system using ab initio and random-phase approximation techniques. Here, our analysis unveils similarities between this novel La 3⁢ Ni 2 ⁢O 7 structure and other Ruddlesden-Popper nickelate superconductors, such as a similar charge-transfer gap value and orbital-selective behavior of the eg orbitals. Pressure primarily increases the bandwidths of the Ni e g bands, suggesting an enhancement of the itinerant properties of those e g states. By changing the cell volume ratio V/V 0 from 0.9 to 1.10, we found that the bilayer structure in La 3 ⁢Ni 2 ⁢O 7 always has lower energy than the single-layer trilayer stacking La 3 ⁢Ni 2 ⁢O 7 . In addition, we observe a “self-doping” effect (compared to the average 1.5 electrons per eg orbital per site of the entire structure) from the trilayer to the single-layer sublattices and this effect will be enhanced by overall electron doping. Moreover, we find a leading d x 2 -y 2 -wave pairing state that is restricted to the single layer. Because the effective coupling between the single layers is very weak, due to the nonsuperconducting trilayer in-between, this suggests that the superconducting transition temperature T c in this structure should be much lower than in the bilayer structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

A galactic approach to neutron scattering science

Neutron scattering science is leading to significant advances in our understanding of materials and will be key to solving many of the challenges that society is facing today. Improvements in scientific instruments are actually making it more difficult to analyze and interpret the results of experiments due to the vast increases in the volume and complexity of data being produced and the associated computational requirements for processing that data. New approaches to enable scientists to leverage computational resources are required, and Oak Ridge National Laboratory (ORNL) has been at the forefront of developing these technologies. We recently completed the design and initial implementation of a neutrons data interpretation platform that allows seamless access to the computational resources provided by ORNL. For the first time, we have demonstrated that this platform can be used for advanced data analysis of correlated quantum materials by utilizing the world's most powerful computer system, Frontier. In particular, we have shown the end-to-end execution of the DCA++ code to determine the dynamic magnetic spin susceptibility χ(q, ω) for a single-band Hubbard model with Coulomb repulsion U/t = 8 in units of the nearest-neighbor hopping amplitude t and an electron density of n = 0.65. The following work describes the architecture, design, and implementation of the platform and how we constructed a correlated quantum materials analysis workflow to demonstrate the viability of this system to produce scientific results.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2024

Topological phase transition without single particle gap closing in strongly correlated systems

Here, in this study, we show two models where changing topology does not necessarily close the bulk insulating charge gap as demanded in the standard noninteracting picture. From extensive determinantal and dynamical cluster quantum Monte Carlo simulations of the half-filled and quarter-filled Kane-Mele-Hubbard model, we show that, for sufficiently strong interactions at either half- or quarter-filling, a transition between topological and trivial insulators occurs without the closing of a charge gap. To shed light on this behavior, we illustrate that an exactly solvable model reveals that while the single-particle gap remains, the many-body gap does, in fact, close. These two gaps are the same in the noninteracting system but depart from each other as the interaction turns on. We purport that for interacting systems, the proper probe of topological phase transitions is the closing of the many-body rather than the single-particle gap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Structural phase transition, s ± -wave pairing, and magnetic stripe order in bilayered superconductor La 3 Ni 2 O 7 under pressure

Motivated by the recently discovered high-T c superconductor La 3 Ni 2 O 7 , we comprehensively study this system using density functional theory and random phase approximation calculations. At low pressures, the Amam phase is stable, containing the Y 2- mode distortion from the Fmmm phase, while the Fmmm phase is unstable. Because of small differences in enthalpy and a considerable Y 2- mode amplitude, the two phases may coexist in the range between 10.6 and 14 GPa, beyond which the Fmmm phase dominates. In addition, the magnetic stripe-type spin order with wavevector (π, 0) was stable at the intermediate region. Pairing is induced in the s ± -wave channel due to partial nesting between the M = (π, π) centered pockets and portions of the Fermi surface centered at the X = (π, 0) and Y = (0, π) points. This resembles results for iron-based superconductors but has a fundamental difference with iron pnictides and selenides. Moreover, our present efforts also suggest La 3 Ni 2 O 7 is qualitatively different from infinite-layer nickelates and cuprate superconductors.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Electronic structure, magnetic correlations, and superconducting pairing in the reduced Ruddlesden-Popper bilayer La 3 Ni 2 O 6 under pressure: Different role of d 3 z 2 - r 2 orbital compared with La 3 Ni 2 O 7

The recent discovery of superconductivity in bilayer La 3 Ni 2 O 7 (327-LNO) under pressure stimulated much interest in layered nickelates. However, superconductivity was not found in another bilayer nickelate system, La 3 Ni 2 O 6 (326-LNO), even under pressure. To understand the similarities and differences between 326-LNO and 327-LNO, using density functional theory and the random phase approximation (RPA), we systematically investigate 326-LNO under pressure. The large crystal-field splitting between the e g orbitals caused by the missing apical oxygen moves the d 3z 2 -r 2 orbital farther away from the Fermi level, implying that the d 3z 2 -r 2 orbital plays a less important role in 326-LNO than in 327-LNO. This also results in a smaller bandwidth for the d x 2 -y 2 orbital and a reduced energy gap for the bonding-antibonding splitting of the d 3z 2 -r 2 orbital in 326-LNO, as compared to 327-LNO. Moreover, the in-plane hybridization between the d x 2 -y 2 and d 3z 2 -r 2 orbitals is found to be small in 326-LNO, while it is much stronger in 327-LNO. Furthermore, the low-spin ferromagnetic state is found to be the likely ground state in 326-LNO under high pressure. The weak interlayer coupling suggests that s ± -wave pairing is unlikely in 326-LNO. The robust in-plane ferromagnetic coupling also suggests that d-wave superconductivity, which is usually caused by antiferromagnetic fluctuations of the d x 2 -y 2 orbital, is also unlikely in 326-LNO. These conclusions are supported by our many-body RPA calculations of the pairing behavior. Additionally, contrasting with the cuprates, for the bilayer cuprate HgBa 2 CaCu 2 O 6 , we find a strong self-doping effect of the d x 2 -y 2 orbital under pressure, with the charge of Cu being reduced by approximately 0.13 electrons from 0 GPa to 25 GPa. In contrast, we do not observe such a change in the electronic density in 326-LNO under pressure, establishing another important difference between the nickelates and the cuprates.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Magnetism and metallicity in moiré transition metal dichalcogenides

The ability to control the properties of twisted bilayer transition metal dichalcogenides in situ makes them an ideal platform for investigating the interplay of strong correlations and geometric frustration. Of particular interest are the low energy scales, which make it possible to experimentally access both temperature and magnetic fields that are of the order of the bandwidth or the correlation scale. In this manuscript, we analyze the moiré Hubbard model, believed to describe the low energy physics of an important subclass of the twisted bilayer compounds. We establish its magnetic and the metal–insulator phase diagram for the full range of magnetic fields up to the fully spin-polarized state. We find a rich phase diagram including fully and partially polarized insulating and metallic phases of which we determine the interplay of magnetic order, Zeeman-field, and metallicity, and make connection to recent experiments.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Trends in electronic structures and s ± -wave pairing for the rare-earth series in bilayer nickelate superconductor R 3 Ni 2 O 7

The recent discovery of pressure-induced superconductivity in the bilayer La 3 Ni 2 O 7 (LNO) has opened a new platform for the study of unconventional superconductors. In this publication, we investigate theoretically the whole family of bilayer 327-type nickelates R 3 Ni 2 O 7 (R = rare-earth elements) under pressure. From La to Lu, the lattice constants and volume decrease, leading to enhanced in-plane and out-of-plane hoppings, resulting in an effectively reduced electronic correlation U / W. Furthermore, the Ni's t 2g states shift away from the e g states, while the crystal-field splitting between d 3z 2 -r 2 and d x 2 -y 2 is almost unchanged. In addition, six candidates were found to become stable in the Fmmm phase, with increasing values of critical pressure as the atomic number increases. Similar to the case of LNO, the s ± -wave pairing tendency dominates in all candidates, due to the nesting between the M = (π , π) and the X = (π , 0) and Y = (0 , π) points in the Brillouin zone. Then, T c is expected to decrease as the radius of rare-earth (RE) ions decreases. In conclusion, our results suggest that LNO is already the “optimal” candidate, with Ce a close competitor, among the whole of the RE bilayer nickelates, and to increase T c we suggest growing on special substrates with larger in-plane lattice spacings.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Weak-coupling theory of neutron scattering as a probe of altermagnetism

Inelastic neutron scattering provides a powerful probe of the magnetic excitations of quantum magnets. Altermagnets have recently emerged as a new class of magnets with vanishing net magnetization characteristic of antiferromagnets and with a spin-split electronic structure typical of ferromagnets. Here we introduce a minimal Hubbard model with two-sublattice orthorhombic anisotropy as a framework to study altermagnetism. Using unrestricted Hartree-Fock calculations, we find an altermagnetic state for this model that evolves from a metallic state to an insulating state with increasing Hubbard-U Coulomb repulsion. We then examine the inelastic neutron scattering response in these states using random-phase approximation calculations of the dynamic spin susceptibility χ"(q,ω). We find that the magnetic excitation spectrum depends on its chirality for q along certain directions in reciprocal space, an observation that may be used in inelastic neutron scattering experiments as a probe of altermagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Spin-singlet topological superconductivity in the attractive Rashba-Hubbard model

Fully gapped, spin-singlet superconductors with antisymmetric spin-orbit coupling in a Zeeman magnetic field provide a promising route to realize superconducting states with non-Abelian topological order and therefore fault-tolerant quantum computation. Here we use a quantum Monte Carlo dynamical cluster approximation to study the superconducting properties of a doped two-dimensional attractive Hubbard model with Rashba spin-orbit coupling in a Zeeman magnetic field. We generally find that the Rashba coupling has a beneficial effect towards s-wave superconductivity. In the presence of a finite Zeeman field, when superconductivity is suppressed by Pauli pair breaking, the Rashba coupling counteracts the spin imbalance created by the Zeeman field by mixing the spins, and thus restores superconductivity at finite temperatures. Further, we show that this favorable effect of the spin-orbit coupling is traced to a spin-flip driven enhancement of the amplitude for the propagation of a pair of electrons in time-reversed states. Moreover, by inspecting the Fermi surface of the interacting model, we show that for sufficiently large Rashba coupling and Zeeman field, the superconducting state is expected to be topologically nontrivial.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Robust charge-density-wave correlations in the electron-doped single-band Hubbard model

There is growing evidence that the hole-doped single-band Hubbard and t–J models do not have a superconducting ground state reflective of the high-temperature cuprate superconductors but instead have striped spin- and charge-ordered ground states. Nevertheless, it is proposed that these models may still provide an effective low-energy model for electron-doped materials. Here we study the finite temperature spin and charge correlations in the electron-doped Hubbard model using quantum Monte Carlo dynamical cluster approximation calculations and contrast their behavior with those found on the hole-doped side of the phase diagram. We find evidence for a charge modulation with both checkerboard and unidirectional components decoupled from any spin-density modulations. These correlations are inconsistent with a weak-coupling description based on Fermi surface nesting, and their doping dependence agrees qualitatively with resonant inelastic x-ray scattering measurements. Our results provide evidence that the single-band Hubbard model describes the electron-doped cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Fluctuating intertwined stripes in the strange metal regime of the Hubbard model

Strongly correlated electron systems host a variety of poorly understood correlations in their high-temperature normal state. Unlike ordered phases defined by order parameters, regions of the normal state are often defined through unconventional properties such as strange metallic transport or spectroscopic pseudogaps. Characterizing the microscopic correlations in the normal state is necessary to elucidate mechanisms that lead to these properties and their connection to ground-state orders. Here, in this paper, we establish the presence of intertwined charge and spin stripes in the strange metal normal state of the Hubbard model using determinant quantum Monte Carlo calculations. The charge and spin density waves constituting the stripes are fluctuating and short ranged; yet they obey a mutual commensurability relation and remain microscopically interlocked, as evidenced through measurements of three-point spin-spin-hole correlation functions. Our findings demonstrate the ability of many-body numerical simulations to unravel the microscopic correlations that define quantum states of matter.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Evidence for chiral superconductivity on a silicon surface

Tin adatoms on a Si(111) substrate with a one-third monolayer coverage form a two-dimensional triangular lattice with one unpaired electron per site. These electrons order into an antiferromagnetic Mott-insulating state, but doping the Sn layer with holes creates a two-dimensional conductor that becomes superconducting at low temperatures. Although the pairing symmetry of the superconducting state is currently unknown, the combination of repulsive interactions and frustration inherent in the triangular adatom lattice opens up the possibility of a chiral order parameter. Here we study the superconducting state of Sn/Si(111) using scanning tunneling microscopy, scanning tunneling spectroscopy and quasiparticle interference imaging. Here we find evidence for a doping-dependent superconducting critical temperature with a fully gapped order parameter, the presence of time-reversal symmetry breaking and a strong enhancement in zero-bias conductance near the edges of the superconducting domains. Although each individual piece of evidence could have a more mundane interpretation, our combined results suggest the possibility that Sn/Si(111) is an unconventional chiral d-wave superconductor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Stripe correlations in the two-dimensional Hubbard-Holstein model

Several state-of-the-art numerical methods have observed static or fluctuating spin and charge stripes in doped two-dimensional Hubbard models, suggesting that these orders play a significant role in shaping the cuprate phase diagram. Many experiments, however, also indicate that the cuprates have strong electron-phonon (e-ph) coupling, and it is unclear how this interaction influences stripe correlations. We study static and fluctuating stripe orders in the doped single-band Hubbard-Holstein model using zero temperature variational Monte Carlo and finite temperature determinant quantum Monte Carlo. We find that the lattice couples more strongly with the charge component of the stripes, leading to an enhancement or suppression of stripe correlations, depending on model parameters like the next-nearest-neighbor hopping t' or phonon energy Ω. Our results help elucidate how the e-ph interaction can tip the delicate balance between stripe and superconducting correlations in the Hubbard-Holstein model with implications for our understanding of the high-T c cuprates.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Enhancing T c in a composite superconductor/metal bilayer system: A dynamical cluster approximation study

It has been proposed that the superconducting transition temperature T c of an unconventional superconductor with a large pairing scale but strong phase fluctuations can be enhanced by coupling it to a metal. However, the general efficacy of this approach across different parameter regimes remains an open question. Using the dynamical cluster approximation, we study this question in a system composed of an attractive Hubbard layer in the intermediate coupling regime, where the magnitude of the attractive Coulomb interaction |U| is slightly larger than the bandwidth W, hybridized with a noninteracting metallic layer. We find that while the superconducting transition becomes more mean-field-like with increasing interlayer hopping, the superconducting transition temperature T c exhibits a nonmonotonic dependence on the strength of the hybridization t ⊥ . Furthermore, this behavior arises from a reduction of the effective pairing interaction in the correlated layer that outcompetes the growth in the intrinsic pair-field susceptibility induced by the coupling to the metallic layer. We find that the largest T c inferred here for the composite system is comparable to the maximum value currently estimated for the isolated negative-U Hubbard model.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Strongly anisotropic electronic and magnetic structures in oxide dichlorides RuOCl 2 and OsOCl 2

The van der Waals oxide dichlorides MOX 2 (M=V, Ta, Nb, Ru, and Os; X=halogen element), with different electronic densities, are attracting considerable attention. Ferroelectricity, spin-singlet formation, and orbital-selective Peierls phases were reported in this family with d 1 or d 2 electronic configurations, all believed to be caused by the strongly anisotropic electronic orbital degree of freedom. Here, using density functional theory and density matrix renormalization group methods, we investigate the electronic and magnetic properties of RuOCl 2 and OsOCl 2 with d 4 electronic configurations. Different from a previous study using VOI 2 with d 1 configuration, these systems with 4d4 or 5d4 do not exhibit a ferroelectric instability along the a axis. Due to the fully occupied dxy orbital in RuOCl 2 and OsOCl 2 , the Peierls instability distortion disappears along the b axis, leading to an undistorted Immm phase (No. 71). Furthermore, we observe strongly anisotropic electronic and magnetic structures along the a axis. For this reason, the materials of our focus can be regarded as “effective one-dimensional” systems even when they apparently have a dominant two-dimensional lattice geometry. The large crystal-field splitting energy (between dxz/yz and dxy orbitals) and large hopping between nearest-neighbor Ru and Os atoms suppresses the J = 0 singlet state in MOCl 2 (M=Ru or Os) with electronic density n = 4, resulting in a spin-1 system. Moreover, we find staggered antiferromagnetic order with π wave vector along the M-O chain direction (a axis) while the magnetic coupling along the b axis is weak. Based on Wannier functions from first-principles calculations, we calculated the relevant hopping amplitudes and crystal-field splitting energies of the t 2g orbitals for the Os atoms to construct a multiorbital Hubbard model for the M-O chains. Staggered AFM with ↑|-|↓-↑|-|↓ spin structure dominates in our density matrix renormalization group calculations, in agreement with density functional theory calculations. Our results for RuOCl 2 and OsOCl 2 provide guidance to experimentalists and theorists working on this interesting family of oxide dichlorides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗