The spontaneous symmetry breaking in Ta2NiSe5 is structural in nature.

The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta2NiSe5 being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals spectroscopic fingerprints that are compatible only with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the gap opening. Our results suggest that the spontaneous symmetry breaking in Ta2NiSe5 is mostly of structural character, hampering the possibility to realize quasi-dissipationless energy transport.

Prediction of unconventional magnetism in doped FeSb2.

It is commonly believed that the energy bands of typical collinear antiferromagnets (AFs), which have zero net magnetization, are Kramers spin-degenerate. Kramers nondegeneracy is usually associated with a global time-reversal symmetry breaking (e.g., via ferromagnetism) or with a combination of spin-orbit interaction and broken spatial inversion symmetry. Recently, another type of spin splitting was demonstrated to emerge in some collinear magnets that are fully spin compensated by symmetry, nonrelativistic, and not even necessarily noncentrosymmetric. These materials feature nonzero spin density staggered in real space as seen in traditional AFs but also spin splitting in momentum space, generally seen only in ferromagnets. This results in a combination of materials characteristics typical of both ferromagnets and AFs. Here, we discuss this recently discovered class with application to a well-known semiconductor, FeSb2, and predict that with certain alloying, it becomes magnetic and metallic and features the aforementioned magnetic dualism. The calculated energy bands split antisymmetrically with respect to spin-degenerate nodal surfaces rather than nodal points, as in the case of spin-orbit splitting. The combination of a large (0.2-eV) spin splitting, compensated net magnetization with metallic ground state, and a specific magnetic easy axis generates a large anomalous Hall conductivity (∼150 S/cm) and a sizable magnetooptical Kerr effect, all deemed to be hallmarks of nonzero net magnetization. We identify a large contribution to the anomalous response originating from the spin-orbit interaction gapped anti-Kramers nodal surfaces, a mechanism distinct from the nodal lines and Weyl points in ferromagnets.

Thermodynamic stability of Li-B-C compounds from first principles.

Prediction of high-Tc superconductivity in hole-doped LixBC two decades ago has brought about an extensive effort to synthesize new materials with honeycomb B-C layers, but the thermodynamic stability of Li-B-C compounds remains largely unexplored. In this study, we use density functional theory to characterize well-established and recently reported Li-B-C phases. Our calculation of the Li chemical potential in LixBC helps estimate the (T,P) conditions required for delithiation of the LiBC parent material, while examination of B-C phases helps rationalize the observation of metastable BC3 polymorphs with honeycomb and diamond-like morphologies. At the same time, we demonstrate that recently reported BC3, LiBC3, and Li2B2C phases with new crystal structures are both dynamically and thermodynamically unstable. With a combination of evolutionary optimization and rational design, we identify considerably more natural and favorable Li2B2C configurations that, nevertheless, remain above the thermodynamic stability threshold.

Assessing the source of error in the Thomas-Fermi-von Weizsäcker density functional.

We investigate the source of error in the Thomas-Fermi-von Weizsäcker (TFW) density functional relative to Kohn-Sham density functional theory (DFT). In particular, through numerical studies on a range of materials, for a variety of crystal structures subject to strain and atomic displacements, we find that while the ground state electron density in TFW orbital-free DFT is close to the Kohn-Sham density, the corresponding energy deviates significantly from the Kohn-Sham value. We show that these differences are a consequence of the poor representation of the linear response within the TFW approximation for the electronic kinetic energy, confirming conjectures in the literature. In so doing, we find that the energy computed from a non-self-consistent Kohn-Sham calculation using the TFW electronic ground state density is in very good agreement with that obtained from the fully self-consistent Kohn-Sham solution.

Unconventional Pressure-Driven Metamagnetic Transitions in Topological van der Waals Magnets.

Activating metamagnetic transitions between ordered states in van der Waals magnets and devices bring great opportunities in spintronics. We show that external pressure, which enhances the interlayer hopping without introducing chemical disorders, triggers multiple metamagnetic transitions upon cooling in the topological van der Waals magnets Mn(Bi1-xSbx)4Te7, where the antiferromagnetic interlayer superexchange coupling competes with the ferromagnetic interlayer coupling mediated by the antisite Mn spins. The temperature-pressure phase diagrams reveal that while the ordering temperature from the paramagnetic to ordered states is almost pressure-independent, the metamagnetic transitions show nontrivial pressure and temperature dependence, even re-entrance. For these highly anisotropic magnets, we attribute the former to the ordering temperature being only weakly dependent on the intralayer parameters and the latter to the parametrically different pressure and temperature dependence of the two interlayer couplings. Our independent probing of these disparate magnetic interactions paves an avenue for efficient magnetic manipulations in van der Waals magnets.

Superconductivity gets an iron boost.

Superconductivity, the resistance-free flow of electrical charges, is one of the most exotic phenomena in solid-state physics. Even though it was discovered almost a century ago, many questions remain unanswered, in particular those concerning the physics of high-temperature superconductivity. The recent discovery of iron-based superconductors was arguably the most important breakthrough in this field for more than two decades and may provide new avenues for understanding this high-temperature phenomenon. Here I present my view of the recent developments in this field that have led to the current understanding of this important new class of superconductor.

Heavy fermions vs doped Mott physics in heterogeneous Ta-dichalcogenide bilayers.

Controlling and understanding electron correlations in quantum matter is one of the most challenging tasks in materials engineering. In the past years a plethora of new puzzling correlated states have been found by carefully stacking and twisting two-dimensional van der Waals materials of different kind. Unique to these stacked structures is the emergence of correlated phases not foreseeable from the single layers alone. In Ta-dichalcogenide heterostructures made of a good metallic "1H"- and a Mott insulating "1T"-layer, recent reports have evidenced a cross-breed itinerant and localized nature of the electronic excitations, similar to what is typically found in heavy fermion systems. Here, we put forward a new interpretation based on first-principles calculations which indicates a sizeable charge transfer of electrons (0.4-0.6 e) from 1T to 1H layers at an elevated interlayer distance. We accurately quantify the strength of the interlayer hybridization which allows us to unambiguously determine that the system is much closer to a doped Mott insulator than to a heavy fermion scenario. Ta-based heterolayers provide therefore a new ground for quantum-materials engineering in the regime of heavily doped Mott insulators hybridized with metallic states at a van der Waals distance.

Ion-Selective Scattering Studied Using the Variable-Energy Electron Irradiation in the Ba0.2K0.8Fe2As2 Superconductor.

Low-temperature variable-energy electron irradiation was used to induce non-magnetic disorder in a single crystal of a hole-doped iron-based superconductor, Ba1-xKxFe2As2, x = 0.80. To avoid systematic errors, the beam energy was adjusted non-consequently for five values between 1.0 and 2.5 MeV when sample resistance was measured in situ at 22 K. For all energies, the resistivity raises linearly with the irradiation fluence suggesting the creation of uncorrelated dilute point-like disorder (confirmed by simulations). The rate of the resistivity increase peaks at energies below 1.5 MeV. Comparison with calculated partial cross-sections points to the predominant creation of defects in the iron sublattice. Simultaneously, superconducting Tc, measured separately between the irradiation runs, is monotonically suppressed as expected, since it depends on the total scattering rate, hence on the total cross-section, which is a monotonically increasing function of the energy. Our work experimentally confirms an often-made assumption of the dominant role of the iron sub-lattice in iron-based superconductors.

Strain-switchable field-induced superconductivity.

Field-induced superconductivity is a rare phenomenon where an applied magnetic field enhances or induces superconductivity. Here, we use applied stress as a control switch between a field-tunable superconducting state and a robust non-field-tunable state. This marks the first demonstration of a strain-tunable superconducting spin valve with infinite magnetoresistance. We combine tunable uniaxial stress and applied magnetic field on the ferromagnetic superconductor Eu(Fe0.88Co0.12)2As2 to shift the field-induced zero-resistance temperature between 4 K and a record-high value of 10 K. We use x-ray diffraction and spectroscopy measurements under stress and field to reveal that strain tuning of the nematic order and field tuning of the ferromagnetism act as independent control parameters of the superconductivity. Combining comprehensive measurements with DFT calculations, we propose that field-induced superconductivity arises from a novel mechanism, namely, the uniquely dominant effect of the Eu dipolar field when the exchange field splitting is nearly zero.

CoTe2 : A Quantum Critical Dirac Metal with Strong Spin Fluctuations.

Quantum critical points separating weak ferromagnetic and paramagnetic phases trigger many novel phenomena. Dynamical spin fluctuations not only suppress the long-range order, but can also lead to unusual transport and even superconductivity. Combining quantum criticality with topological electronic properties presents a rare and unique opportunity. Here, by means of ab initio calculations and magnetic, thermal, and transport measurements, it is shown that the orthorhombic CoTe2 is close to ferromagnetism, which appears suppressed by spin fluctuations. Calculations and transport measurements reveal nodal Dirac lines, making it a rare combination of proximity to quantum criticality and Dirac topology.

Nontrivial Doping Evolution of Electronic Properties in Ising-Superconducting Alloys.

Transition metal dichalcogenides offer unprecedented versatility to engineer 2D materials with tailored properties to explore novel structural and electronic phase transitions. In this work, the atomic-scale evolution of the electronic ground state of a monolayer of Nb1- δ Moδ Se2 across the entire alloy composition range (0 < δ < 1) is investigated using low-temperature (300 mK) scanning tunneling microscopy and spectroscopy (STM/STS). In particular, the atomic and electronic structure of this 2D alloy throughout the metal to semiconductor transition (monolayer NbSe2 to MoSe2 ) is studied. The measurements enable extraction of the effective doping of Mo atoms, the bandgap evolution and the band shifts, which are monotonic with δ. Furthermore, it is demonstrated that collective electronic phases (charge density wave and superconductivity) are remarkably robust against disorder and further shown that the superconducting TC changes non-monotonically with doping. This contrasting behavior in the normal and superconducting state is explained using first-principles calculations. Mo doping is shown to decrease the density of states at the Fermi level and the magnitude of pair-breaking spin fluctuations as a function of Mo content. These results paint a detailed picture of the electronic structure evolution in 2D TMD alloys, which is of utmost relevance for future 2D materials design.

Field-tunable toroidal moment in a chiral-lattice magnet.

Ferrotoroidal order, which represents a spontaneous arrangement of toroidal moments, has recently been found in a few linear magnetoelectric materials. However, tuning toroidal moments in these materials is challenging. Here, we report switching between ferritoroidal and ferrotoroidal phases by a small magnetic field, in a chiral triangular-lattice magnet BaCoSiO4 with tri-spin vortices. Upon applying a magnetic field, we observe multi-stair metamagnetic transitions, characterized by equidistant steps in the net magnetic and toroidal moments. This highly unusual ferri-ferroic order appears to come as a result of an unusual hierarchy of frustrated isotropic exchange couplings revealed by first principle calculations, and the antisymmetric exchange interactions driven by the structural chirality. In contrast to the previously known toroidal materials identified via a linear magnetoelectric effect, BaCoSiO4 is a qualitatively new multiferroic with an unusual coupling between several different orders, and opens up new avenues for realizing easily tunable toroidal orders.

Direct-Write of Nanoscale Domains with Tunable Metamagnetic Order in FeRh Thin Films.

We have directly written nanoscale patterns of magnetic ordering in FeRh films using focused helium-ion beam irradiation. By varying the dose, we pattern arrays with metamagnetic transition temperatures that range from the as-grown film temperature to below room temperature. We employ transmission electron microscopy, X-ray diffraction, and temperature-dependent transport measurements to characterize the as-grown film, and magneto-optic Kerr effect imaging to quantify the He+ irradiation-induced changes to the magnetic order. Moreover, we demonstrate temperature-dependent optical microscopy and conductive atomic force microscopy as indirect probes of the metamagnetic transition that are sensitive to the differences in dielectric properties and electrical conductivity, respectively, of FeRh in the antiferromagnetic (AF) and ferromagnetic (FM) states. Using density functional theory, we quantify strain- and defect-induced changes in spin-flip energy to understand their influence on the metamagnetic transition temperature. This work holds promise for in-plane AF-FM spintronic devices, by reducing the need for multiple patterning steps or different materials, and potentially eliminating interfacial polarization losses due to cross material interfacial spin scattering.

Density functional theory-based electric field gradient database.

The deviation of the electron density around the nuclei from spherical symmetry determines the electric field gradient (EFG), which can be measured by various types of spectroscopy. Nuclear Quadrupole Resonance (NQR) is particularly sensitive to the EFG. The EFGs, and by implication NQR frequencies, vary dramatically across materials. Consequently, searching for NQR spectral lines in previously uninvestigated materials represents a major challenge. Calculated EFGs can significantly aid at the search's inception. To facilitate this task, we have applied high-throughput density functional theory calculations to predict EFGs for 15187 materials in the JARVIS-DFT database. This database, which will include EFG as a standard entry, is continuously increasing. Given the large scope of the database, it is impractical to verify each calculation. However, we assess accuracy by singling out cases for which reliable experimental information is readily available and compare them to the calculations. We further present a statistical analysis of the results. The database and tools associated with our work are made publicly available by JARVIS-DFT ( https://www.ctcms.nist.gov/~knc6/JVASP.html ) and NIST-JARVIS API ( http://jarvis.nist.gov/ ).

Double Indirect Interlayer Exciton in a MoSe2/WSe2 van der Waals Heterostructure.

An emerging class of semiconductor heterostructures involves stacking discrete monolayers such as transition metal dichalcogenides (TMDs) to form van der Waals heterostructures. In these structures, it is possible to create interlayer excitons (ILEs), spatially indirect, bound electron-hole pairs with the electron in one TMD layer and the hole in an adjacent layer. We are able to clearly resolve two distinct emission peaks separated by 24 meV from an ILE in a MoSe2/WSe2 heterostructure fabricated using state-of-the-art preparation techniques. These peaks have nearly equal intensity, indicating they are of common character, and have opposite circular polarizations when excited with circularly polarized light. Ab initio calculations successfully account for these observations: they show that both emission features originate from excitonic transitions that are indirect in momentum space and are split by spin-orbit coupling. Also, the electron is strongly hybridized between both the MoSe2 and WSe2 layers, with significant weight in both layers, contrary to the commonly assumed model. Thus, the transitions are not purely interlayer in character. This work represents a significant advance in our understanding of the static and dynamic properties of TMD heterostructures.