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At least 1,027 records · Page 57
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DOE OSTI2022

Inverse Faraday effect in Mott insulators

The inverse Faraday effect (IFE), where a static magnetization is induced by circularly polarized light, offers a promising route to ultrafast control of spin states. Here we study the IFE in Mott insulators using the Floquet theory. We find two distinct IFE behavior governed by the inversion symmetry. In the Mott insulators with inversion symmetry, we find that the effective magnetic field induced by the IFE couples ferromagnetically to the neighboring spins. While for the Mott insulators without inversion symmetry, the effective magnetic field due to IFE couples antiferromagnetically to the neighboring spins. We apply the theory to the spin-orbit coupled single- and multiorbital Hubbard model that is relevant for the Kitaev quantum spin liquid material and demonstrate that the magnetic interactions can be tuned by light.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Magnetic interactions of 4 f electrons in the topological insulator chalcogenide Bi 2 Se 3

Here, the gap opening mechanism of a topological insulator, the quantum anomalous Hall effect and the axion physics are still pressing open questions and a microscopic viewpoint to further understand the role of magnetism in topology is highly desirable. In this work we have performed a micro scopic investigation, by means of electron spin resonance (ESR) along with complementary bulk measurements, on the chalcogenide (Bi 1-x Gd x ) 2 Se 3 (x = 0, 0.001, 0.002 and 0.006). Our analysis of the Gd 3+ spin dynamics reveal no significant change of the Fermi surface as a function of Gd 3+ concentration, which indicates that the 4f magnetism is different from the non-local effects induced by transition metals (d electrons) substitutions. Additionally, we observe an unusual evolution of the Gd 3+ ESR spectra as a function of the applied magnetic field, which we discuss considering the magnetic interaction between Gd 3+ 4f electrons and impurity centers such as Se vacancies. This interaction would give rise to a local weak antilocalization effect surrounding the Gd 3+ ions. Such mechanism is observable due to particular details of the Gd 3+ 4f electrons magnetism in this system compared to d electrons. Our work points out that rare earth substitutions in this model topological insulator is a promising path to explore the axion insulating systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Symmetry breaking forms split-off flat bands in quantum oxides controlling metal versus insulator phases

The crystal structure used as input to electronic structure calculation of conventionally bonded solids consists primarily of the standard crystallographic degrees of freedom. Quantum solids sometimes have additional microscopic degrees of freedom (m-DOF) nested within the crystallographic structure. These might include local motifs including positional (Peierls dimers, deformed octahedra, Jahn-Teller distortions), magnetic (local moment configurations) and dipolar (local ferroelectric configurations). Such motifs can be observed experimentally via local probes that avoid averaging, and theoretically as distinct total energy lowering features relative to more simplified “average crystallographic structures”. Here we examine the ability of electronic structure methods independent of strong correlation physics to explain the broad phenomenology of metal-insulator selectivity in quantum oxides by energy-lowering symmetry breaking. We do this by avoiding the restriction of considering only (i) electron-electron interactions in a fixed unresponsive lattice—as done in Mott strong correlation explanations—allowing, however, (ii) local positional and magnetic motifs that coexist within a crystallographic landscape. We find in a broad range of quantum oxides with different symmetry breaking modes the formation of split-off flat bands that can also control metallic versus insulating characteristics. The split-off band effect is common to magnetic and non-magnetic materials, including both binary and ternary oxides. One finds that when such local symmetry breaking motifs are considered in mean-field-like (e.g. density functional theory) electronic structure calculations of quantum oxides, they explain many of the observed trends in metal vs insulator phases discussed otherwise in prior literature via strong correlation in symmetry unbroken view.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2012

Spin-orbit tuned metal-insulator transitions in single-crystal Sr₂Ir 1–x Rh x O₄ (0≤x≤1)

Sr₂IrO₄ is a magnetic insulator driven by spin-orbit interaction (SOI) whereas the isoelectronic and isostructural Sr₂RhO₄ is a paramagnetic metal. The contrasting ground states have been shown to result from the critical role of the strong SOI in the iridate. Our investigation of structural, transport, magnetic, and thermal properties reveals that substituting 4d Rh⁴⁺ (4d⁵) ions for 5d Ir⁴⁺ (5d⁵) ions in Sr₂IrO₄ directly reduces the SOI and rebalances the competing energies so profoundly that it generates a rich phase diagram for Sr₂Ir 1–x Rh x O₄ featuring two major effects: (1) Light Rh doping (0 ≤ x ≤ 0.16) prompts a simultaneous and precipitous drop in both the electrical resistivity and the magnetic ordering temperature TC, which is suppressed to zero at x = 0.16 from 240 K at x = 0. (2) However, with heavier Rh doping [0.24 < x < 0.85 (±0.05)] disorder scattering leads to localized states and a return to an insulating state with spin frustration and exotic magnetic behavior that only disappears near x = 1. The intricacy of Sr₂Ir 1–x Rh x O₄ is further highlighted by comparison with Sr₂Ir 1–x Ru x O₄ where Ru⁴⁺ (4d⁴) drives a direct crossover from the insulating to metallic states.

Qi, T. F.↗
DOE OSTI2015

Fully gapped superconductivity in In-doped topological crystalline insulator Pb 0.5 Sn 0.5 Te

In this study, superconductors derived from topological insulators and topological crystalline insulators by chemical doping have long been considered to be candidates as topological superconductors. Pb 0.5 Sn 0.5 Te is a topological crystalline insulator with mirror symmetry protected surface states on (001)-, (011)-, and (111)-oriented surfaces. The superconductor (Pb 0.5 Sn 0.5 ) 0.7 In 0.3 Te is produced by In doping in Pb 0.5 Sn 0.5 Te, and is thought to be a topological superconductor. Here we report scanning tunneling spectroscopy measurements of the superconducting state as well as the superconducting energy gap in (Pb 0.5 Sn 0.5 ) 0.7 In 0.3 Te on a (001)-oriented surface. The spectrum can be well fitted by an anisotropic s-wave gap function of Δ = 0.72 + 0.18cos4θ meV using Dynes model. The results show that the superconductor seems to be a fully gapped one without any in-gap states, in contradiction with the expectation of a topological superconductor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Percolative metal-insulator transition in LaMnO 3

In this work, we show that the pressure-induced metal-insulator transition (MIT) in LaMnO 3 is fundamentally different from the Mott-Hubbard transition and is percolative in nature, with the measured resistivity obeying the percolation scaling laws. Using the Gutzwiller method to treat correlation effects in a model Hamiltonian that includes both Coulomb and Jahn-Teller interactions, we show, one, that the MIT is driven by a competition between electronic correlation and the electron-lattice interaction, an issue that has been long debated, and two, that with compressed volume, the system has a tendency towards phase separation into insulating and metallic regions, consisting, respectively, of Jahn-Teller distorted and undistorted octahedra. This tendency manifests itself in a mixed phase of intermixed insulating and metallic regions in the experiment. Conduction in the mixed phase occurs by percolation and the MIT occurs when the metallic volume fraction, steadily increasing with pressure, exceeds the percolation threshold v c ≈ 0.29. Finally, measured high-pressure resistivity follows the percolation scaling laws quite well, and the temperature dependence follows the Efros-Shklovskii variable-range hopping behavior for granular materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Changes in the electronic structure and spin dynamics across the metal-insulator transition in LaLa 1-x Sr x CoO 3

The magnetoelectronic properties of La 1-x Sr x CoO 3 , which include giant magnetoresistance, are strongly dependent on the level of hole doping. The system evolves, with increasing x, from a spin glass insulator to a metallic ferromagnet with a metal-insulator (MI) transition at x C ~ 0.18. Nanoscale phase separation occurs in the insulating phase and persists, to some extent, into the just-metallic phase. The present experiments at 4.2 K have used 139 La NMR to investigate the transition from hopping dynamics for x < x C to Korringa-like ferromagnetic metal behavior for x > x C . A marked decrease in the spin-lattice relaxation rate is found in the vicinity of x C as the MI transition is crossed. Lastly, this behavior is accounted for in terms of the evolution of the electronic structure and dynamics with cluster size.

36 MATERIALS SCIENCE↗
DOE OSTI2017

BaSn 2 : A wide-gap strong topological insulator

BaSn 2 has been shown to form as layers of buckled stanene intercalated by barium ions. However, despite an apparently straightforward synthesis and significant interest in stanene as a topological material, BaSn 2 has been left largely unexplored, and has only recently been recognized as a potential topological insulator. Belonging to neither the lead nor bismuth chalcogenide families, it would represent a unique manifestation of the topological insulating phase. Here in this paper, we present a detailed investigation of BaSn 2 , using both ab initio and experimental methods. First-principles calculations demonstrate that this overlooked material is indeed a strong, wide-gap topological insulator with a bulk band gap of 200 meV. We characterize the surface state dependence on termination chemistry, providing guidance for experimental efforts to measure and manipulate its topological properties. Additionally, through ab initio modeling and synthesis experiments, we explore the stability and accessibility of this phase, revealing a complicated phase diagram that indicates a challenging path to obtaining single crystals.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Robust antiferromagnetic spin waves across the metal-insulator transition in hole-doped BaMn 2 As 2

BaMn 2 As 2 is an antiferromagnetic insulator where a metal-insulator transition occurs with hole doping via the substitution of Ba with K. The metal-insulator transition causes only a small suppression of the Néel temperature (T N ) and the ordered moment, suggesting that doped holes interact weakly with the Mn spin system. Powder inelastic neutron scattering measurements were performed on three different samples of Ba 1 - x K x Mn 2 As 2 with x = 0 , 0.125, and 0.25 to study the effect of hole doping and metallization on the spin dynamics. We compare the neutron intensities to a linear spin-wave theory approximation to the J 1 $-$ J 2 $-$ J c Heisenberg model. Hole doping is found to introduce only minor modifications to the exchange energies and spin gap. Lastly, the changes observed in the exchange constants are consistent with the small drop of T N with doping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Magnetic field dependent dynamics and field-driven metal-to-insulator transition of the half-filled Hubbard model: A DMFT+DMRG study

Here, we study the magnetic field-driven metal-to-insulator transition in half-filled Hubbard model on the Bethe lattice, using the dynamical mean-field theory by solving the quantum impurity problem with density-matrix renormalization group algorithm. The method enables us to obtain a high-resolution spectral densities in the presence of a magnetic field. It is found that the Kondo resonance at the Fermi level splits at relatively high magnetic field: the spin-up and -down components move away from the Fermi level and finally form a spin-polarized band insulator. By calculating the magnetization and spin susceptibility, we clarify that an applied magnetic field drives a transition from a paramagnetic metallic phase to a band insulating phase. In the weak interaction regime, the nature of the transition is continuous and captured by the Stoner's description, while in the strong interaction regime the transition is very likely to be metamagnetic, evidenced by the hysteresis curve. Furthermore, we determine the phase boundary by tracking the kink in the magnetic susceptibility, and the steplike change of the entanglement entropy and the entanglement gap closing. Interestingly, the phase boundaries determined from these two different ways are largely consistent with each other.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Influence of magnetism and correlation on the spectral properties of doped Mott insulators

Unraveling the nature of the doping-induced transition between a Mott insulator and a weakly correlated metal is crucial to understanding novel emergent phases in strongly correlated materials. Here, for this purpose, we study the evolution of spectral properties upon doping Mott insulating states by utilizing the cluster perturbation theory on the Hubbard and t – J -like models. Specifically, a quasifree dispersion crossing the Fermi level develops with small doping, and it eventually evolves into the most dominant feature at high doping levels. Although this dispersion is related to the free-electron hopping, our study shows that this spectral feature is, in fact, influenced inherently by both electron-electron correlation and spin-exchange interaction: the correlation destroys coherence, while the coupling between spin and mobile charge restores it in the photoemission spectrum. Due to the persistent impact of correlations and spin physics, the onset of gaps or the high-energy anomaly in the spectral functions can be expected in doped Mott insulators.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Large Spin-Wave Bullet in a Ferrimagnetic Insulator Driven by the Spin Hall Effect

Due to its transverse nature, spin Hall effects (SHE) provide the possibility to excite and detect spin currents and magnetization dynamics even in magnetic insulators. Magnetic insulators are outstanding materials for the investigation of nonlinear phenomena and for novel low power spintronics applications because of their extremely low Gilbert damping. Here, we report on the direct imaging of electrically driven spin-torque ferromagnetic resonance (ST-FMR) in the ferrimagnetic insulator Y 3 Fe 5 O 12 based on the excitation and detection by SHEs. The driven spin dynamics in Y 3 Fe 5 O 12 is directly imaged by spatially-resolved microfocused Brillouin light scattering (BLS) spectroscopy. Previously, ST-FMR experiments assumed a uniform precession across the sample, which is not valid in our measurements. A strong spin-wave localization in the center of the sample is observed indicating the formation of a nonlinear, self-localized spin-wave `bullet'.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Correlation-driven insulator-metal transition in near-ideal vanadium dioxide films

We use polarization- and temperature-dependent x-ray absorption spectroscopy, in combination with photoelectron microscopy, x-ray diffraction, and electronic transport measurements, to study the driving force behind the insulator-metal transition in VO 2 . We show that both the collapse of the insulating gap and the concomitant change in crystal symmetry in homogeneously strained single-crystalline VO 2 films are preceded by the purely electronic softening of Coulomb correlations within V-V singlet dimers. Furthermore, this process starts 7 K (±0.3 K) below the transition temperature, as conventionally defined by electronic transport and x-ray diffraction measurements, and sets the energy scale for driving the near-room-temperature insulator-metal transition in this technologically promising material.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Two-Dimensional J eff = 1 / 2 Antiferromagnetic Insulator Unraveled from Interlayer Exchange Coupling in Artificial Perovskite Iridate Superlattices

We report an experimental investigation of the two-dimensional J eff =1/2 antiferromagnetic Mott insulator by varying the interlayer exchange coupling in [(SrIrO 3 ) 1 , (SrTiO 3 ) m ] (m=1, 2 and 3) superlattices. Although all samples exhibited an insulating ground state with long-range magnetic order, temperature-dependent resistivity measurements showed a stronger insulating behavior in the m = 2 and m = 3 samples than the m = 1 sample which displayed a clear kink at the magnetic transition. This difference indicates that the blocking effect of the excessive SrTiO 3 layer enhances the effective electron-electron correlation and strengthens the Mott phase. The significant reduction of the Néel temperature from 150 K for m = 1 to 40 K for m = 2 demonstrates that the long-range order stability in the former is boosted by a substantial interlayer exchange coupling. Resonant x-ray magnetic scattering revealed that the interlayer exchange coupling has a switchable sign, depending on the SrTiO 3 layer number m, for maintaining canting-induced weak ferromagnetism. In conclusion, the nearly unaltered transition temperature between the m = 2 and the m = 3 demonstrated that we have realized a two-dimensional antiferromagnet at finite temperatures with diminishing interlayer exchange coupling.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Engineering an Insulating Ferroelectric Superlattice with a Tunable Band Gap from Metallic Components

The recent discovery of “polar metals” with ferroelectriclike displacements offers the promise of designing ferroelectrics with tunable energy gaps by inducing controlled metal-insulator transitions. Here in this work, we employ first-principles calculations to design a metallic polar superlattice from nonpolar metal components and show that controlled intermixing can lead to a true insulating ferroelectric with a tunable band gap. We consider a 2/2 superlattice made of two centrosymmetric metallic oxides, La 0.75 Sr 0.25 MnO 3 and LaNiO 3 , and show that ferroelectriclike displacements are induced. The ferroelectriclike distortion is found to be strongly dependent on the carrier concentration (Sr content). Further, we show that a metal-to-insulator (MI) transition is feasible in this system via disproportionation of the Ni sites. Such a disproportionation and, hence, a MI transition can be driven by intermixing of transition metal ions between Mn and Ni layers. Finally, as a result, the energy gap of the resulting ferroelectric can be tuned by varying the degree of intermixing in the experimental fabrication method.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Response of the Lattice across the Filling-Controlled Mott Metal-Insulator Transition of a Rare Earth Titanate

The lattice response of a prototype Mott insulator, SmTiO 3 , to hole doping is investigated with atomic-scale spatial resolution. SmTiO 3 films are doped with Sr on the Sm site with concentrations that span the insulating and metallic sides of the filling-controlled Mott metal-insulator transition (MIT). The GdFeO 3 -type distortions are investigated using an atomic resolution scanning transmission electron microscopy technique that can resolve small lattice distortions with picometer precision. We show that these distortions are gradually and uniformly reduced as the Sr concentration is increased without any phase separation. Significant distortions persist into the metallic state. In conclusion, the results present a new picture of the physics of this prototype filling-controlled MIT, which is discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Unexpected Intermediate State Photoinduced in the Metal-Insulator Transition of Submicrometer Phase-Separated Manganites

At ultrafast timescales, the initial and final states of a first-order metal-insulator transition often coexist forming clusters of the two phases. In this work, we report an unexpected third long-lived intermediate state emerging at the photoinduced first-order metal-insulator transition of La 0.325 Pr 0.3 Ca 0.375 MnO 3 , known to display submicrometer length-scale phase separation. Using magnetic force microscopy and time-dependent magneto-optical Kerr effect, we determined that the third state is a nanoscale mixture of the competing ferromagnetic metallic and charge-ordered insulating phases, with its own physical properties. This discovery bridges the two different families of colossal magnetoresistant manganites known experimentally and shows for the first time that the associated states predicted by theory can coexist in a single sample.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Half-Excitonic Insulator: A Single-Spin Bose-Einstein Condensate

First-principles calculations reveal an unusual electronic state (dubbed as half excitonic insulator) in monolayer 1T-MX2 (M = Co, Ni and X = Cl, Br). Its one spin channel has a many-body ground state due to excitonic instability, while the other is characterized by a conventional band insulator gap. This disparity arises from a competition between the band gap and exciton binding energy, which exhibits a spin-dependence due to different orbital occupations. Such a state can be identified by optical absorption measurements and angle-resolved photoemission spectroscopy. Finally, our theory not only provides new insights for the study of exciton condensation in magnetic materials but also suggests that strongly correlated materials could be fertile candidates for excitonic insulators.

36 MATERIALS SCIENCE↗