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At least 325 records · Page 18

Embracing disorder in quantum materials design

Many of the most exciting materials discoveries in fundamental condensed matter physics are made in systems hosting some degree of intrinsic disorder. While disorder has historically been regarded as something to be avoided in materials design, it is often of central importance to correlated and quantum materials. This is largely driven by the conceptual and theoretical ease to handle, predict, and understand highly uniform systems that exhibit complex interactions, symmetries, and band structures. In this Perspective, we highlight how flipping this paradigm has enabled exciting possibilities in the emerging field of high entropy materials, focusing primarily on high entropy oxide and chalcogenide quantum materials. These materials host high levels of cation or anion compositional disorder while maintaining unexpectedly uniform single crystal lattices. The diversity of atomic scale interactions of spin, charge, orbital, and lattice degrees of freedom are found to emerge into coherent properties on much larger length scales. Thus, altering the variance and magnitudes of the atomic scale properties through elemental selection can open new routes to tune global correlated phases, such as magnetism, metal–insulator transitions, ferroelectricity, and even emergent topological responses. The strategy of embracing disorder in this way provides a much broader pallet from which functional states can be designed for next-generation microelectronic and quantum information systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetoelastic effects in the hyperhoneycomb Kitaev spin liquid

In recent years, several magnetic Mott insulators with strong spin-orbit coupling were suggested to be proximate to the Kitaev quantum spin liquid, whose one of the most exciting features is the fractionalization of spin excitations into itinerant Majorana fermions and static Z 2 fluxes. Unfortunately, the ground states of these systems cannot be easily captured by experiment, remaining featureless to conventional local probes. Here, we propose to study the signatures of fractionalized excitations by exploiting their coupling to the lattice vibrations, dubbed magnetoelastic coupling, which arises from the fact that the interaction between spins depends on the relative distance between them. We argue that the magnetoelastic coupling can lead to the distinct modification of the phonon dynamics, which can be observed by measuring renormalized phonon spectrum, the sound attenuation, and the phonon Hall viscosity. This makes the phonon dynamics a promising tool for the characterization and identification of quantum spin liquid phases. In this work, we focus on the magnetoelastic effects in the three-dimensional Kitaev model realized on the hyperhoneycomb lattice. Here, the hyperhoneycomb Kitaev spin liquid is particularly interesting since the strong Kitaev interaction was observed in the Kitaev magnet β-Li 2 IrO 3 , for which the spin-orbit entangled J eff = 1/2 moments of iridium ions form precisely the hyperhoneycomb lattice.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis and electronic properties of Nd n +1 NinO 3 n +1 Ruddlesden-Popper nickelate thin films

The rare-earth nickelates possess a diverse set of collective phenomena including metal-to-insulator transitions, magnetic phase transitions, and, upon chemical reduction, superconductivity. In this work, we demonstrate epitaxial stabilization of layered nickelates in the Ruddlesden-Popper form, Nd n +1 NinO 3 n +1 , using molecular beam epitaxy. By optimizing the stoichiometry of the parent perovskite NdNiO 3 , we can reproducibly synthesize the n = 1–5 member compounds. X-ray absorption spectroscopy at the O K and Ni L edges indicate systematic changes in both the nickel-oxygen hybridization level and nominal nickel filling from 3$d^8$ to 3$d^7$ as we move across the series from n = 1 to n = ∞. The n = 3 – 5 compounds exhibit weakly hysteretic metal-to-insulator transitions with transition temperatures that depress with increasing order toward NdNiO 3 ( n = ∞).

36 MATERIALS SCIENCE↗

Probing Ice-Rule-Breaking Transition in Dy 2 Ti 2 O 7 Thin Film by Proximitized Transport and Magnetic Torque

While the spin-ice state of bulk pyrochlores such as Dy 2⁢ Ti 2 ⁢O 7 and Ho 2⁢ Ti 2 ⁢O 7 has been extensively studied in the past several decades due to its unique degenerate ground state and emergent monopole excitation, whether it survives in the thin-film form remains a mystery. The limited volume of the thin-film sample makes it challenging to study the intrinsic magnetic properties. Here, we synthesized 18-nm-thick Dy 2⁢ Ti 2 ⁢O 7 thin film on yttria-stabilized zirconia with 9.5 mol% Y 2 ⁢O 3 substrate and capped it by a thin conductive Bi 2 ⁢Ir 2 ⁢O 7 layer and performed the proximitized magnetoresistance measurements. Our Letter found that the ice-rule-breaking phase transition survives but with a modified effective nearest-neighbor interaction (𝐽 eff =1.054 K) and distorted Ising spin axes (𝜀 = +0.051) compared to the bulk crystal. Furthermore, the results are supported by the simultaneously measured capacitive torque magnetometry. Our Letter demonstrates that proximitized transport is an effective tool for thin films of insulating frustrated magnets.

Magnetic interactions↗

Bottom-Up Soft Magnetic Composites

In order to meet 2025 goals for enhanced peak power (100 kW), specific power (50 kW/L), and reduced cost (3.3 $/kW) in a motor that can operate at ≥ 20,000 rpm, improved soft magnetic materials must be developed. Better performing soft magnetic materials will also enable electric motors without rare earth elements. In fact, replacement of permanent magnets with soft magnetic materials was highlighted in the Electrical and Electronics Technical Team (EETT) Roadmap as a R&D pathway for meeting 2025 targets. Eddy current losses in conventional soft magnetic materials, such as silicon steel, begin to significantly impact motor efficiency as rotational speed is increased. Soft magnetic composites (SMCs), which combine magnetic particles with an insulating matrix to boost electrical resistivity (ρ) and decrease eddy current losses, even at higher operating frequencies (or rotational speeds), are an attractive solution. Today, SMCs are being fabricated with values of ρ ranging between 10 -3 to 10 -1 μohm∙m, which is significantly higher than 3% silicon steel (~0.5 μohm∙m). The isotropic nature of SMCs is ideally suited for motors with 3D flux paths, such as axial flux motors. Additionally, the manufacturing cost of SMCs is low and they are highly amenable to advanced manufacturing and net-shaping into complex geometries, which further reduces manufacturing costs. There is still significant room for advancement in SMCs, and therefore additional improvements in electrical machine performance. For example, despite the inclusion of a non-magnetic insulating material, the electrical resistivities of SMCs are still far below that of soft ferrites (10 – 10 8 μohm∙m).

36 MATERIALS SCIENCE↗

Electric Drive Technologies Research: Bottom-Up Soft Magnetic Composites (FY2022 Annual Progress Report)

In order to meet 2025 goals for enhanced peak power (100 kW), specific power (50 kW/L), and reduced cost (3.3 $\$$/kW) in a motor that can operate at ≥ 20,000 rpm, improved soft magnetic materials must be developed. Better performing soft magnetic materials will also enable rare earth free electric motors. In fact, replacement of permanent magnets with soft magnetic materials was highlighted in the Electrical and Electronics Technical Team (EETT) Roadmap as a R&D pathway for meeting 2025 targets. Eddy current losses in conventional soft magnetic materials, such as silicon steel, begin to significantly impact motor efficiency as rotational speed increases. Soft magnetic composites (SMCs), which combine magnetic particles with an insulating matrix to boost electrical resistivity (ρ) and decrease eddy current losses, even at higher operating frequencies (or rotational speeds), are an attractive solution. Today, SMCs are being fabricated with values of ρ ranging between 10 -3 to 10 -1 μohm∙m, which is significantly higher than 3% silicon steel (~0.05 μohm∙m). The isotropic nature of SMCs is ideally suited for motors with 3D flux paths, such as axial flux motors. Additionally, the manufacturing cost of SMCs is low and they are highly amenable to advanced manufacturing and net-shaping into complex geometries, which further reduces manufacturing costs. There is still significant room for advancement in SMCs, and therefore additional improvements in electrical machine performance. For example, despite the inclusion of a non-magnetic insulating material, the electrical resistivities of SMCs are still far below that of soft ferrites (10 – 10 8 μohm∙m).

33 ADVANCED PROPULSION SYSTEMS↗

Two-step electronic response to magnetic ordering in a van der Waals ferromagnet

The two-dimensional material Cr 2 ⁢Ge 2 ⁢Te 6 is a member of the class of insulating van der Waals (vdW) magnets. Here, using high resolution angle-resolved photoemission spectroscopy in a detailed temperature dependence study, we identify a clear response of the electronic structure to a dimensional crossover in the form of two distinct temperature scales marking onsets of modifications in the electronic structure. Specifically, we observe Te 𝑝-orbital-dominated bands to undergo changes at the Curie transition temperature 𝑇 𝐶 while the Cr 𝑑-orbital-dominated bands begin evolving at a higher temperature scale. Combined with neutron scattering, density functional theory calculations, and Monte Carlo simulations, we find that the electronic system can be consistently understood to respond sequentially to the distinct temperatures at which in-plane and out-of-plane spin correlations exceed a characteristic length scale. Finally, our findings reveal the sensitivity of the orbital-selective electronic structure for probing the dynamical evolution of local moment correlations in vdW insulating magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Procedures for Assessing the Stability of Proposed Topological Materials

Here, we investigate the stability of MnPb 2 Bi 2 Te 6 (MPBT), which is predicted to be a magnetic topological insulator (TI), using density functional theory calculations. Our analysis includes various measures such as enthalpies of formation, Helmholtz free energies, defect formation energies, and dynamical stability. Our thermodynamic analysis shows that the phonon contribution to the energy gain from finite temperature is estimated to be less than 10 meV/atom, which may not be sufficient to stabilize MPBT at high temperatures, even with the most favorable reactions starting from binaries. While MPBT is generally robust against the formation of various defects, we find that the anti-site defect formation of MnPb is the most likely to occur, with a corresponding energy less than 60 meV. This can be attributed to the significant energy cost from compressive strain at the PbTe layer. Our findings suggest that MPBT is on the brink of stability in terms of thermodynamics and defect formation, underscoring the importance of conducting systematic analyses of the stability of proposed TIs, including MPBT, for their practical utilization. This study offers valuable insights into the design and synthesis of desirable magnetic TI materials with robust stabilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrical Manipulation of Topological Phases in a Quantum Anomalous Hall Insulator

Quantum anomalous Hall phases arising from the inverted band topology in magnetically doped topological insulators have emerged as an important subject of research for quantization at zero magnetic fields. Though necessary for practical implementation, sophisticated electrical control of molecular beam epitaxy (MBE)-grown quantum anomalous Hall matter have been stymied by growth and fabrication challenges. Here, in this study, a novel procedure is demonstrated, employing a combination of thin-film deposition and 2D material stacking techniques, to create dual-gated devices of the MBE-grown quantum anomalous Hall insulator, Cr-doped (Bi,Sb) 2 Te 3 . In these devices, orthogonal control over the field-induced charge density and the electric displacement field is demonstrated. A thorough examination of material responses to tuning along each control axis is presented, realizing magnetic property control along the former and a novel capability to manipulate the surface exchange gap along the latter. Through electrically addressing the exchange gap, the capabilities to either strengthen the quantum anomalous Hall state or suppress it entirely and drive a topological phase transition to a trivial state are demonstrated. The experimental result is explained using first principle theoretical calculations, and establishes a practical route for in situ control of quantum anomalous Hall states and topology.

36 MATERIALS SCIENCE↗

Universal Magnetic Phases in Twisted Bilayer MoTe 2

Twisted bilayer MoTe 2 (tMoTe 2 ) has emerged as a robust platform for exploring correlated topological phases, yet the evolution of its magnetism and topology with twist angle remains an open question. Here, we systematically map the magnetic phase diagram of tMoTe 2 by using local optical spectroscopy and scanning nanoSQUID-on-tip magnetometry. We identify spontaneous ferromagnetism at filling factors ν = −1 and −3 across twist angles from 2.1° to 3.7°, revealing a universal, twist-angle-insensitive ferromagnetic phase. At 2.1°, we further observe robust ferromagnetism at ν = −5, absent at larger twist angles. Temperature-dependent measurements reveal a contrasting twist-angle dependence of the Curie temperatures between ν = −1 and −3, indicating a distinct interplay between the exchange interactions and bandwidth for the two Chern bands. Despite broken time-reversal symmetry, no topological gap is detected at ν = −3. Furthermore, our results establish a global framework for understanding and controlling magnetic order in tMoTe 2 .

Insulators↗

Observation of coherently coupled cation spin dynamics in an insulating ferrimagnetic oxide

Many technologically useful magnetic oxides are ferrimagnetic insulators, which consist of chemically distinct cations. In this work, we examine the spin dynamics of different magnetic cations in ferrimagnetic NiZnAl-ferrite (Ni 0.65 Zn 0.35 Al 0.8 Fe 1.2 O 4 ) under continuous microwave excitation. Specifically, we employ time-resolved x-ray ferromagnetic resonance to separately probe Fe 2+/3+ and Ni 2+ cations on different sublattice sites. Our results show that the precessing cation moments retain a rigid, collinear configuration to within ≈2°. Moreover, the effective spin relaxation is identical to within <10% for all magnetic cations in the ferrite. Thus, we validate the oft-assumed “ferromagnetic-like” dynamics in the resonantly driven ferrimagnetic oxide: the magnetic moments from different cations precess as a coherent, collective magnetization, despite the high contents of nonmagnetic Zn 2+ and Al 3+ diluting the exchange interactions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Stacking Faults and Topological Properties in MnBi 2 Te 4 : Reconciling Gapped and Gapless States

Despite theoretical predictions of a gapped surface state for the magnetic topological insulator MnBi 2 Te 4 (MBT), there has been a series of experimental evidence pointing toward gapless states. Here, we theoretically explore how stacking faults could influence the topological characteristics of MBT. We envisage a scenario that a stacking fault exists at the surface of MBT, causing the uppermost layer to deviate from the ground state and its interlayer separation to be expanded. This stacking fault with modulated interlayer couplings hosts a nearly gapless state within the topmost layer due to charge redistribution as the outermost layer recedes. Furthermore, we find evidence of spin-momentum locking and preservation of weak band inversion in the gapless surface state, suggesting the nontrivial topological surface states in the presence of the stacking fault. In conclusion, our findings provide a plausible elucidation to the long-standing conundrum of reconciling the observation of gapped and gapless states on MBT surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Topological surface currents accessed through reversible hydrogenation of the three-dimensional bulk

Hydrogen, the smallest and most abundant element in nature, can be efficiently incorporated within a solid and drastically modify its electronic and structural state. In most semiconductors interstitial hydrogen binds to defects and is known to be amphoteric, namely it can act either as a donor (H + ) or an acceptor (H - ) of charge, nearly always counteracting the prevailing conductivity type. Here we demonstrate that hydrogenation resolves an outstanding challenge in chalcogenide classes of three-dimensional (3D) topological insulators and magnets — the control of intrinsic bulk conduction that denies access to quantum surface transport, imposing severe thickness limits on the bulk. With electrons donated by a reversible binding of H + ions to Te(Se) chalcogens, carrier densities are reduced by over 10 20 cm -3 , allowing tuning the Fermi level into the bulk bandgap to enter surface/edge current channels without altering carrier mobility or the bandstructure. The hydrogen-tuned topological nanostructures are stable at room temperature and tunable disregarding bulk size, opening a breadth of device platforms for harnessing emergent topological states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-throughput predictions of metal–organic framework electronic properties: theoretical challenges, graph neural networks, and data exploration

Abstract With the goal of accelerating the design and discovery of metal–organic frameworks (MOFs) for electronic, optoelectronic, and energy storage applications, we present a dataset of predicted electronic structure properties for thousands of MOFs carried out using multiple density functional approximations. Compared to more accurate hybrid functionals, we find that the widely used PBE generalized gradient approximation (GGA) functional severely underpredicts MOF band gaps in a largely systematic manner for semi-conductors and insulators without magnetic character. However, an even larger and less predictable disparity in the band gap prediction is present for MOFs with open-shell 3 d transition metal cations. With regards to partial atomic charges, we find that different density functional approximations predict similar charges overall, although hybrid functionals tend to shift electron density away from the metal centers and onto the ligand environments compared to the GGA point of reference. Much more significant differences in partial atomic charges are observed when comparing different charge partitioning schemes. We conclude by using the dataset of computed MOF properties to train machine-learning models that can rapidly predict MOF band gaps for all four density functional approximations considered in this work, paving the way for future high-throughput screening studies. To encourage exploration and reuse of the theoretical calculations presented in this work, the curated data is made publicly available via an interactive and user-friendly web application on the Materials Project.

36 MATERIALS SCIENCE↗

Graphene bilayers with a twist

Near a magic twist angle, bilayer graphene transforms from a weakly correlated Fermi liquid to a strongly correlated two-dimensional electron system with properties that are extraordinarily sensitive to carrier density and to controllable environmental factors such as the proximity of nearby gates and twist-angle variation. Among other phenomena, magic-angle twisted bilayer graphene hosts superconductivity, interaction-induced insulating states, magnetism, electronic nematicity, linear-in-temperature low-temperature resistivity and quantized anomalous Hall states. Here, we highlight some key research results in this field, point to important questions that remain open and comment on the place of magic-angle twisted bilayer graphene in the strongly correlated quantum matter world.

36 MATERIALS SCIENCE↗

The role of iron in magnetic damping of Mg(Al,Fe) 2 O 4 spinel ferrite thin films

© 2020 Author(s). We have investigated magnesium aluminum ferrite thin films with a range of iron concentrations and identified the optimal iron content to obtain high crystalline quality thin films with the low magnetic damping required for spin current-based applications. Epitaxial MgAl 2-x FexO4 films with 0.8 < x < 2.0 were grown by pulsed laser deposition on single crystal MgAl2O4 substrates and were characterized structurally and magnetically. We find that the x = 1.5 composition minimizes the room-temperature magnetic damping with a typical Gilbert damping parameter of α eff = 1.8 × 10-3. This minimized damping is governed by a competition between the more robust magnetic ordering with increased iron content, x, and the more defective structure due to larger film-substrate lattice mismatch with increased iron content. The temperature-dependent magnetization curves indicate that Tc is suppressed below room temperature for iron content x ≤ 1.2 and eventually suppressed entirely for x = 0.8. X-ray magnetic circular dichroism results indicate that for all x the magnetic moment is dominated by Fe 3 + cations distributed in a 60:40 ratio on the octahedral and tetrahedral sites, with minimal contribution from Fe 2 + cations. Films with x = 1.4-1.6 exhibit very strong ferromagnetic resonance and low Gilbert damping with α eff = (1.8-6) × 10-3, making them ideal candidates for microwave and spintronic applications.

36 MATERIALS SCIENCE↗

Theory of magnon polaritons in quantum Ising materials

Here, we present a theory of magnon-polaritons in quantum Ising materials, and develop a formalism describing the coupling between light and matter as an Ising system is tuned through its quantum critical point. The theory is applied to Ising materials having multilevel single-site Hamiltonians, in which multiple magnon modes are present, such as the insulating Ising magnet LiHoF 4 . We find that the magnon-photon coupling strengths may be tuned by the applied transverse field, with the coupling between the soft mode present in the quantum Ising material and a photonic resonator mode diverging at the quantum critical point of the material. A fixed system of spins will not exhibit the diamagnetic response expected when light is coupled to mobile spins or atoms. Without the diamagnetic response, one expects a divergent magnon-photon coupling strength to lead to a superradiant quantum phase transition. However, this neglects the effects of damping and decoherence present in any real system. We show that damping and decoherence may block the superradiant quantum phase transition, and lead to weak coupling between the soft magnon mode and the resonator mode. The results of the theory are applied to experimental data on the model system LiHoF 4 in a microwave resonator.

74 ATOMIC AND MOLECULAR PHYSICS↗