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At least 937 records · Page 52

Emergent Phenomena in Oxide Nanostructures

The field of oxide electronics has seen tremendous growth over two decades and oxide materials find wide-ranging applications in information storage, fuel cells, batteries, and more. Phase transitions, such as magnetic and metal-to-insulator transitions, are one of the most important phenomena in oxide nanostructures. Many novel devices utilizing these phase transitions have been proposed, ranging from ultrafast switches for logic applications to low power memory structures. Yet, despite this promise and many years of research, a complete understanding of phase transitions in oxide nanostructures remains elusive. In this LDRD, we report two important observations of phase transitions. We conducted a systematic study of these transitions. Moreover, emergent quantum phenomena due to the strong correlations and interactions among the charge, orbital, and spin degrees of freedom inherent in transition metal oxides were explored. In addition, a new, fast atomic-scale chemical imaging technique developed through the characterization of these oxides is presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observation of cyclotron antiresonance in the topological insulator Bi 2 Te 3

Here, we report on the experimental observation of a cyclotron antiresonance in a canonical three-dimensional topological insulator Bi 2 Te 3 . Magnetoreflectance response of single-crystal Bi 2 Te 3 was studied in 18-T magnetic field, and compared to other topological insulators studied before, the main spectral feature is inverted. We refer to it as an antiresonance. In order to describe this unconventional behavior we propose the idea of an imaginary cyclotron resonance frequency, which on the other hand indicates that the form of the Lorentz force that magnetic field exerts on charge carriers takes an unconventional form.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Enhancement of interlayer exchange in an ultrathin two-dimensional magnet

Following the recent isolation of monolayer CrI 3 , many more two-dimensional van der Waals magnetic materials have been isolated. Their incorporation in van der Waals heterostructures offers a new platform for spintronics, proximity magnetism and quantum spin liquids. A primary question in this field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies of CrI 3 have shown a different magnetic ground state for ultrathin exfoliated films compared with the bulk, but the origin is not yet understood. Here, we use electron tunnelling through few-layer crystals of the layered antiferromagnetic insulator CrCl 3 to probe its magnetic order and find a tenfold enhancement of the interlayer exchange compared with bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveals that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low-temperature stacking order and, we hypothesize, increased interlayer exchange. In conclusion, our study provides insight into the connection between stacking order and interlayer interactions in two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets such as RuCl 3 .

36 MATERIALS SCIENCE↗

Tunneling Planar Hall Effect in Topological Insulators: Spin Valves and Amplifiers

We investigate tunneling across a single ferromagnetic barrier on the surface of a three-dimensional topological insulator. In the presence of a magnetization component along the bias direction, a tunneling planar Hall conductance (TPHC), transverse to the applied bias, develops. Electrostatic control of the barrier enables a giant Hall angle, with the TPHC exceeding the longitudinal tunneling conductance. By changing the in-plane magnetization direction, it is possible to change the sign of both the longitudinal and transverse differential conductance without opening a gap in the topological surface state. The transport in a topological-insulator–ferromagnet junction can, thus, be drastically altered from a simple spin valve to an amplifier.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Reversible hydrogen control of antiferromagnetic anisotropy in α-Fe 2 O 3

Antiferromagnetic insulators are a ubiquitous class of magnetic materials, holding the promise of low-dissipation spin-based computing devices that can display ultra-fast switching and are robust against stray fields. However, their imperviousness to magnetic fields also makes them difficult to control in a reversible and scalable manner. Here we demonstrate a novel proof-of-principle ionic approach to control the spin reorientation (Morin) transition reversibly in the common antiferromagnetic insulator α-Fe 2 O 3 (haematite) - now an emerging spintronic material that hosts topological antiferromagnetic spin-textures and long magnon-diffusion lengths. We use a low-temperature catalytic-spillover process involving the post-growth incorporation or removal of hydrogen from α-Fe 2 O 3 thin films. Hydrogenation drives pronounced changes in its magnetic anisotropy, Néel vector orientation and canted magnetism via electron injection and local distortions. We explain these effects with a detailed magnetic anisotropy model and first-principles calculations. Tailoring our work for future applications, we demonstrate reversible control of the room-temperature spin-state by doping/expelling hydrogen in Rh-substituted α-Fe 2 O 3 .

36 MATERIALS SCIENCE↗

Direct experimental evidence of tunable charge transfer at the LaNiO 3 / CaMnO 3 ferromagnetic interface

Interfacial charge transfer in oxide heterostructures gives rise to a rich variety of electronic and magnetic phenomena. Designing heterostructures where one of the thin-film components exhibits a metal-insulator transition opens a promising avenue for controlling such phenomena both statically and dynamically. In this work, we utilize a combination of depth-resolved soft x-ray standing-wave and hard x-ray photoelectron spectroscopies in conjunction with polarization-dependent x-ray absorption spectroscopy to investigate the effects of the metal-insulator transition in LaNiO 3 on the electronic and magnetic states at the LaNiO 3 /CaMnO 3 interface. Here, we report a direct observation of the reduced effective valence state of the interfacial Mn cations in the metallic superlattice with an above-critical LaNiO 3 thickness (6 unit cells, u.c.) facilitated by the charge transfer of itinerant Ni 3d e g electrons into the interfacial CaMnO 3 layer. Conversely, in an insulating superlattice with a below-critical LaNiO 3 thickness of 2 u.c., a homogeneous effective valence state of Mn is observed throughout the CaMnO 3 layers due to the blockage of charge transfer across the interface. The ability to switch and tune interfacial charge transfer enables precise control of the emergent ferromagnetic state at the LaNiO 3 /CaMnO 3 interface and, thus, has far-reaching consequences on the future strategies for the design of next-generation spintronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Metal-insulator transition in (111) SrRuO 3 ultrathin films

(111)-oriented transition metal oxide thin films provide a route to developing oxide-based topological quantum materials, but the epitaxial growth is challenging. Here, we present the thickness-dependent electronic and magnetic phase diagrams of coherently strained, phase pure (111)-oriented SrRuO 3 epitaxial films grown on (111) SrTiO 3 substrates using pulsed laser deposition. With decreasing film thickness, it is found that both the metal-to-insulator and magnetic phase transitions occur at the same thickness of 4–5 nm for films grown along both the (111) and the (001) directions. The character of the transport near the metal-insulator transition is, however, distinct for the different directions, which is attributed to the increased electron-electron correlation for (111) SrRuO 3 . The results presented here illustrate both the broad challenges as well as the possibilities in modifying correlated materials using dimensional tuning of electronic and magnetic properties.

36 MATERIALS SCIENCE↗

Magnetization Dependent In-plane Anomalous Hall Effect in a Low-dimensional System

Anomalous Hall Effect (AHE) response in magnetic systems is typically proportional to an out-of-plane magnetization component because of the restriction imposed by system symmetries, which demands that the magnetization, applied electric field, and induced Hall current are mutually orthogonal to each other. Here, we report experimental realization of an unconventional form of AHE in a low-dimensional heterostructure, wherein the Hall response is not only proportional to the out-of-plane magnetization component but also to the in-plane magnetization component. By interfacing a low-symmetry topological semimetal (TaIrTe4) with the ferromagnetic insulator (Cr2Ge2Te6), we create a low-dimensional magnetic system, where only one mirror symmetry is preserved. We show that as long as the magnetization has a finite component in the mirror plane, this last mirror symmetry is broken, allowing the emergence of an AHE signal proportional to in-plane magnetization. Our experiments, conducted on multiple devices, reveal a gate-voltage-dependent AHE response, suggesting that the underlying mechanisms responsible for the Hall effect in our system can be tuned via electrostatic gating. A minimal microscopic model constrained by the symmetry of the heterostructure shows that both interfacial spin-orbit coupling and time-reversal symmetry breaking via the exchange interaction from magnetization are responsible for the emergence of the in-plane AHE. Our work highlights the importance of system symmetries and exchange interaction in low-dimensional heterostructures for designing novel and tunable Hall effects in layered quantum systems.

FOS: Physical sciences↗

Electronic fingerprints of Cr and V dopants in the topological insulator Sb 2 Te 3

By combining scanning tunneling microscopy/spectroscopy and first-principles calculations, we systematically study the local electronic states of magnetic dopants V and Cr in the topological insulator (TI) Sb 2 Te 3 . Spectroscopic imaging shows diverse local defect states between Cr and V, which agree with our first-principle calculations. The unique spectroscopic features of V and Cr dopants provide electronic fingerprints for the codoped magnetic TI samples with the enhanced quantum anomalous Hall effect. Here our results also facilitate the exploration of the underlying mechanism of the enhanced quantum anomalous Hall temperature in Cr/V codoped TIs.

36 MATERIALS SCIENCE↗

Absence of a Dirac gap in ferromagnetic Cr x (Bi 0.1 Sb 0.9 ) 2-x Te 3

Magnetism breaks the time-reversal symmetry expected to open a Dirac gap in 3D topological insulators that consequently leads to the quantum anomalous Hall effect. The most common approach of inducing a ferromagnetic state is by doping magnetic 3d elements into the bulk of 3D topological insulators. In Cr 0.15 (Bi 0.1 Sb 0.9 ) 1.85 Te 3 , the material where the quantum anomalous Hall effect was initially discovered at temperatures much lower than the ferromagnetic transition, T C , the scanning tunneling microscopy studies have reported a large Dirac gap of ~20–100 meV. The discrepancy between the low temperature of quantum anomalous Hall effect (< C ) and large spectroscopic Dirac gaps (>>T C ) found in magnetic topological insulators remains puzzling. Here, we used angle-resolved photoemission spectroscopy to study the surface electronic structure of the pristine and potassium doped surface of Cr 0.15 (Bi 0.1 Sb 0.9 ) 1.85 Te 3 . Upon potassium deposition, the p-type surface state of the pristine sample was turned into an n-type, allowing the spectroscopic observation of Dirac point. Finally, we find a gapless surface state, with no evidence of a large Dirac gap reported in tunneling studies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Novel Phases and Dynamics of Multi-orbital Mott Insulators

The goal of this project is to gain theoretical insight into magnetism in the presence of spin-orbit coupling (SOC) for multi-orbital Mott insulators. Inspired by the exact solution of the Kitaev model that harbors a quantum spin liquid with novel excitations and struck by its relevance for materials with anisotropic orbital interactions, the PI will explore various new classes of 4d and 5d transition metal oxides. Starting with all electron Hamiltonians, the PI will derive minimal magnetic models. The aim will be to understand the role played by orbital frustration, even in the absence of any geometric frustration, in creating orbitally ordered as well as spin-orbital liquid phases. Orbital frustration arises primarily from the directional or anisotropic nature of d-orbitals in contrast to the isotropic nature of the spin degree of freedom. These models will be investigated by a variety of theoretical and numerical methods, including exact diagonalization, mean field theories, density matrix renormalization group and quantum Monte Carlo methods. Testable predictions for three experiments: nuclear magnetic resonance (NMR) and resonant x-ray scattering (RXS) to probe orbital ordering and pump-probe experiments to probe quantum dynamics will test the validity of these models for materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ionic Tuning of Cobaltites at the Nanoscale

Control of materials through custom design of ionic distributions is one of the most promising approaches for developing future technologies ranging from spintronic logic and memory devices to energy storage. Perovskites have shown particular promise for ionic-devices due to their high ion mobility and sensitivity to chemical stoichiometry. In this work, we demonstrate control of ion distributions in (La,Sr)CoO3. Commensurate with control of the oxygen stoichiometry, the Co valence and saturation magnetization show a smooth continuous variation. In contrast, magnetoresistance measurements show a sharp, step-wise transition in the magnetic anisotropy and resistivity over the same range of oxygen stoichiometry. These results suggest significant phase separation, with conductive magnetic regions and oxygen-deficient, insulating, non-magnetic regions, forming percolated networks. Indeed, X-ray diffraction identifies oxygen vacancy ordering, including the emergence of Brownmillerite ordering. The unusual appearance of the Brownmillerite phase under ambient temperature is further confirmed by high resolution scanning transmission electron microscopy. This work demonstrates room-temperature ionic control of magnetism, electrical conductivity and crystalline structure, in a 40 nm film, presenting new opportunities for ionic devices that leverage multiple material properties.

thin films, magnetism, xmcd, pnr, STEM, defects↗

Magnetic order driven ultrafast phase transition in NdNiO 3

Ultrashort x-ray pulses can be used to disentangle magnetic and structural dynamics and are accordingly utilized here to study the photoexcitation of NdNiO 3 (NNO), a model nickelate exhibiting structural and magnetic dynamics that conspire to induce an insulator-to-metal transition (IMT). Here, during the course of the photoinduced IMT with above-gap excitation, we observe an ultrafast (< 180 fs) quenching of magnetic order followed by a time delayed collapse of the insulating phase probed by x-ray absorption and THz transmission (450 fs) that correlates with the slowest optical phonon mode involved in the structural transition. A simultaneous order-disorder response at the Ni site and displacive response at the Nd site coexist in the ultrafast magnetic response. Crucially, we observe the optical phonon through its coherent coupling with Nd magnetic order, demonstrating that the magnetic and structural degrees of freedom both contribute in driving the IMT. Density functional theory calculations reveal a consistent scenario where optically driven intersite charge transfer drives a collapse of antiferromagnetic order that in turn destabilizes the charge-ordered phase resulting in an IMT. These experiments provide different modalities for the control of electronic phase transitions in quantum materials based on the ultrafast interplay between structural and magnetic orders created by femtosecond photoexcitation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Experimental evidence for nonspherical magnetic form factor in Ru 3 +

The Mott insulator ..alpha..-RuCl3 has generated great interest in the community due to its possible field-induced Kitaev quantum spin liquid state. Despite enormous effort spent trying to obtain the form of the low-energy Hamiltonian, there is currently no agreed upon set of parameters which is able to explain all of the data. A key piece of missing information lies in the determination of the magnetic form factor of Ru3+, particularly for a true quantitative treatment of inelastic neutron scattering data. Here we present the experimentally derived magnetic form factor of Ru3+ in the low spin 4d5 state using polarized neutron diffraction within the paramagnetic regime on high-quality single crystals of ..alpha..-RuCl3. We observe strong evidence of an anisotropic form factor, expected of the spin-orbit coupled jeff=12 ground state. We model the static magnetization density in increasing complexity from simple isotropic cases, to a multipolar expansion, and, finally, ab initio calculations of the generalized jeff=12 ground state. Comparison of both single ion models and inclusion of Cl- anions support the presence of hybridization of Ru3+ with the surrounding Cl- ligands.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Matrix-type effect on the magnetotransport properties of Ni–AlO and Ni–NbO composite systems

The effect of the insulating-matrix material on the electronic and magnetic properties of nanocomposites is investigated in the Ni{sub x}(Al{sub 2}O{sub 3}){sub 100–x} metal–insulator system and the Ni{sub x}(Nb{sub 2}O{sub 5}){sub 100–x} metal–semiconductor system. It is established that the characteristics of composites determined by electron transport through the matrix (the electrical resistivity, the position of the electrical percolation threshold, the magnetoresistance effect) depend on the material type. Replacement of the matrix from Al{sub 2}O{sub 3} to Nb{sub 2}O{sub 5} results in a decrease in the electrical resistivity by two–three orders of magnitude, a decrease in the magnetic resistivity by more than an order of magnitude, and in displacement of the percolation threshold from 40 to 30 at % of Ni. In this case, the magnetic properties of the composites are independent of the type of matrix: the concentration of the magnetic percolation threshold is identical in the two systems (~45 at % of Ni), and the coercive force of the samples occurring beyond the percolation threshold is close in magnitude (5–8 and 12–18 Oe) in the Ni{sub x}(Nb{sub 2}O{sub 5}){sub 100–x} and Ni{sub x}(Al{sub 2}O{sub 3}){sub 100–x} composites, respectively.

36 MATERIALS SCIENCE↗

Quantum Hall edge states in topological insulator nanoribbons

We present a microscopic theory of the chiral one-dimensional electron gas system localized on the sidewalls of magnetically doped Bi 2 Se 3 -family topological insulator nanoribbons in the quantum anomalous Hall effect (QAHE) regime. Our theory is based on a simple continuum model of sidewall states whose parameters are extracted from detailed ribbon and film geometry tight-binding model calculations. In contrast to the familiar case of the quantum Hall effect in semiconductor quantum wells, the number of microscopic chiral channels depends simply and systematically on the ribbon thickness and on the position of the Fermi level within the surface state gap. Further, we use our theory to interpret recent transport experiments that exhibit nonzero longitudinal resistance in samples with accurately quantized Hall conductances.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tunable correlated Chern insulator and ferromagnetism in a moiré superlattice

Studies of two-dimensional electron systems in a strong magnetic field revealed the quantum Hall effect, a topological state of matter featuring a finite Chern number C and chiral edge states. Haldane later theorized that Chern insulators with integer quantum Hall effects could appear in lattice models with complex hopping parameters even at zero magnetic field. The ABC-trilayer graphene/hexagonal boron nitride (ABC-TLG/hBN) moiré superlattice provides an attractive platform with which to explore Chern insulators because it features nearly flat moiré minibands with a valley-dependent, electrically tunable Chern number. In this work, we report the experimental observation of a correlated Chern insulator in an ABC-TLG/hBN moiré superlattice. We show that reversing the direction of the applied vertical electric field switches the moiré minibands of ABC-TLG/hBN between zero and finite Chern numbers, as revealed by large changes in magneto-transport behaviour. For topological hole minibands tuned to have a finite Chern number, we focus on quarter filling, corresponding to one hole per moiré unit cell. The Hall resistance is well quantized at h/2e 2 (where h is Planck’s constant and e is the charge on the electron), which implies C = 2, for a magnetic field exceeding 0.4 tesla. The correlated Chern insulator is ferromagnetic, exhibiting substantial magnetic hysteresis and a large anomalous Hall signal at zero magnetic field. Finally, our discovery of a C = 2 Chern insulator at zero magnetic field should open up opportunities for discovering correlated topological states, possibly with topological excitations, in nearly flat and topologically nontrivial moiré minibands.

36 MATERIALS SCIENCE↗

Robust odd-parity superconductivity in the doped topological insulator Nb x Bi 2 Se 3

We present resistivity and magnetization measurements on proton-irradiated crystals demonstrating that the superconducting state in the doped topological insulator Nb x Bi 2 Se 3 (x = 0.25) is surprisingly robust against disorder-induced electron scattering. The superconducting transition temperature T c decreases without indication of saturation with increasing defect concentration, and the corresponding scattering rates far surpass expectations based on conventional theory. The low-temperature variation of the London penetration depth Δλ(T) follows a power law [Δλ(T)~T 2 ] indicating the presence of symmetry-protected point nodes. Lastly, our results are consistent with the proposed robust nematic E u pairing state in this material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗