*Nat Commun ; 14(1): 5852, 2023 Sep 20.*

##### RESUMO

Understanding the nature and origin of collective excitations in materials is of fundamental importance for unraveling the underlying physics of a many-body system. Excitation spectra are usually obtained by measuring the dynamical structure factor, S(Q, ω), using inelastic neutron or x-ray scattering techniques and are analyzed by comparing the experimental results against calculated predictions. We introduce a data-driven analysis tool which leverages 'neural implicit representations' that are specifically tailored for handling spectrographic measurements and are able to efficiently obtain unknown parameters from experimental data via automatic differentiation. In this work, we employ linear spin wave theory simulations to train a machine learning platform, enabling precise exchange parameter extraction from inelastic neutron scattering data on the square-lattice spin-1 antiferromagnet La2NiO4, showcasing a viable pathway towards automatic refinement of advanced models for ordered magnetic systems.

*Science ; 381(6654): 181-186, 2023 Jul 14.*

##### RESUMO

Quantum geometry in condensed-matter physics has two components: the real part quantum metric and the imaginary part Berry curvature. Whereas the effects of Berry curvature have been observed through phenomena such as the quantum Hall effect in two-dimensional electron gases and the anomalous Hall effect (AHE) in ferromagnets, the quantum metric has rarely been explored. Here, we report a nonlinear Hall effect induced by the quantum metric dipole by interfacing even-layered MnBi2Te4 with black phosphorus. The quantum metric nonlinear Hall effect switches direction upon reversing the antiferromagnetic (AFM) spins and exhibits distinct scaling that is independent of the scattering time. Our results open the door to discovering quantum metric responses predicted theoretically and pave the way for applications that bridge nonlinear electronics with AFM spintronics.

*ACS Nano ; 17(11): 10164-10171, 2023 Jun 13.*

##### RESUMO

Recent experiments report a charge density wave (CDW) in the antiferromagnet FeGe, but the nature of the charge ordering and the associated structural distortion remains elusive. We discuss the structural and electronic properties of FeGe. Our proposed ground state phase accurately captures atomic topographies acquired by scanning tunneling microscopy. We show that the 2 × 2 × 1 CDW likely results from the Fermi surface nesting of hexagonal-prism-shaped kagome states. FeGe is found to exhibit distortions in the positions of the Ge atoms instead of the Fe atoms in the kagome layers. Using in-depth first-principles calculations and analytical modeling, we demonstrate that this unconventional distortion is driven by the intertwining of magnetic exchange coupling and CDW interactions in this kagome material. The movement of Ge atoms from their pristine positions also enhances the magnetic moment of the Fe kagome layers. Our study indicates that magnetic kagome lattices provide a material candidate for exploring the effects of strong electronic correlations on the ground state and their implications for transport, magnetic, and optical responses in materials.

*Nat Commun ; 14(1): 2228, 2023 Apr 19.*

##### RESUMO

The spacetime light cone is central to the definition of causality in the theory of relativity. Recently, links between relativistic and condensed matter physics have been uncovered, where relativistic particles can emerge as quasiparticles in the energy-momentum space of matter. Here, we unveil an energy-momentum analogue of the spacetime light cone by mapping time to energy, space to momentum, and the light cone to the Weyl cone. We show that two Weyl quasiparticles can only interact to open a global energy gap if they lie in each other's energy-momentum dispersion cones-analogous to two events that can only have a causal connection if they lie in each other's light cones. Moreover, we demonstrate that the causality of surface chiral modes in quantum matter is entangled with the causality of bulk Weyl fermions. Furthermore, we identify a unique quantum horizon region and an associated 'thick horizon' in the emergent causal structure.

*Nat Mater ; 22(5): 583-590, 2023 May.*

##### RESUMO

Using circularly polarized light to control quantum matter is a highly intriguing topic in physics, chemistry and biology. Previous studies have demonstrated helicity-dependent optical control of chirality and magnetization, with important implications in asymmetric synthesis in chemistry; homochirality in biomolecules; and ferromagnetic spintronics. We report the surprising observation of helicity-dependent optical control of fully compensated antiferromagnetic order in two-dimensional even-layered MnBi2Te4, a topological axion insulator with neither chirality nor magnetization. To understand this control, we study an antiferromagnetic circular dichroism, which appears only in reflection but is absent in transmission. We show that the optical control and circular dichroism both arise from the optical axion electrodynamics. Our axion induction provides the possibility to optically control a family of [Formula: see text]-symmetric antiferromagnets ([Formula: see text], inversion; [Formula: see text], time-reversal) such as Cr2O3, even-layered CrI3 and possibly the pseudo-gap state in cuprates. In MnBi2Te4, this further opens the door for optical writing of a dissipationless circuit formed by topological edge states.

*Nature ; 617(7961): 493-498, 2023 May.*

##### RESUMO

Photocathodes-materials that convert photons into electrons through a phenomenon known as the photoelectric effect-are important for many modern technologies that rely on light detection or electron-beam generation1-3. However, current photocathodes are based on conventional metals and semiconductors that were mostly discovered six decades ago with sound theoretical underpinnings4,5. Progress in this field has been limited to refinements in photocathode performance based on sophisticated materials engineering1,6. Here we report unusual photoemission properties of the reconstructed surface of single crystals of the perovskite oxide SrTiO3(100), which were prepared by simple vacuum annealing. These properties are different from the existing theoretical descriptions4,7-10. In contrast to other photocathodes with a positive electron affinity, our SrTiO3 surface produces, at room temperature, discrete secondary photoemission spectra, which are characteristic of efficient photocathode materials with a negative electron affinity11,12. At low temperatures, the photoemission peak intensity is enhanced substantially and the electron beam obtained from non-threshold excitations shows longitudinal and transverse coherence that differs from previous results by at least an order of magnitude6,13,14. The observed emergence of coherence in secondary photoemission points to the development of a previously undescribed underlying process in addition to those of the current theoretical photoemission framework. SrTiO3 is an example of a fundamentally new class of photocathode quantum materials that could be used for applications that require intense coherent electron beams, without the need for monochromatic excitations.

*Phys Rev Lett ; 130(4): 046402, 2023 Jan 27.*

##### RESUMO

The interplay of nontrivial topology and superconductivity in condensed matter physics gives rise to exotic phenomena. However, materials are extremely rare where it is possible to explore the full details of the superconducting pairing. Here, we investigate the momentum dependence of the superconducting gap distribution in a novel Dirac material PdTe. Using high resolution, low temperature photoemission spectroscopy, we establish it as a spin-orbit coupled Dirac semimetal with the topological Fermi arc crossing the Fermi level on the (010) surface. This spin-textured surface state exhibits a fully gapped superconducting Cooper pairing structure below T_{c}â¼4.5 K. Moreover, we find a node in the bulk near the Brillouin zone boundary, away from the topological Fermi arc. These observations not only demonstrate the band resolved electronic correlation between topological Fermi arc states and the way it induces Cooper pairing in PdTe, but also provide a rare case where surface and bulk states host a coexistence of nodeless and nodal gap structures enforced by spin-orbit coupling.

*Nano Lett ; 23(3): 902-907, 2023 Feb 08.*

##### RESUMO

Magnetic materials exhibiting topological Dirac fermions are attracting significant attention for their promising technological potential in spintronics. In these systems, the combined effect of the spin-orbit coupling and magnetic order enables the realization of novel topological phases with exotic transport properties, including the anomalous Hall effect and magneto-chiral phenomena. Herein, we report experimental signature of topological Dirac antiferromagnetism in TaCoTe2 via angle-resolved photoelectron spectroscopy and first-principles density functional theory calculations. In particular, we find the existence of spin-orbit coupling-induced gaps at the Fermi level, consistent with the manifestation of a large intrinsic nonlinear Hall conductivity. Remarkably, we find that the latter is extremely sensitive to the orientation of the Néel vector, suggesting TaCoTe2 as a suitable candidate for the realization of non-volatile spintronic devices with an unprecedented level of intrinsic tunability.

*Adv Mater ; : e2201058, 2022 Nov 22.*

##### RESUMO

Interest in topological materials continues to grow unabated in view of their conceptual novelties as well as their potential as platforms for transformational new technologies. Electronic states in a topological material are robust against perturbations and support unconventional electromagnetic responses. The first-principles band-theory paradigm has been a key player in the field by providing successful prediction of many new classes of topological materials. This perspective presents a cross section through the recent work on understanding the role of geometry and topology in generating topological states and their responses to external stimuli, and as a basis for connecting theory and experiment within the band theory framework. In this work, effective strategies for topological materials discovery and impactful directions for future topological materials research are also commented.

*Nat Commun ; 13(1): 6046, 2022 Oct 20.*

##### RESUMO

In one-dimensional (1D) systems, electronic interactions lead to a breakdown of Fermi liquid theory and the formation of a Tomonaga-Luttinger Liquid (TLL). The strength of its many-body correlations can be quantified by a single dimensionless parameter, the Luttinger parameter K, characterising the competition between the electrons' kinetic and electrostatic energies. Recently, signatures of a TLL have been reported for the topological edge states of quantum spin Hall (QSH) insulators, strictly 1D electronic structures with linear (Dirac) dispersion and spin-momentum locking. Here we show that the many-body interactions in such helical Luttinger Liquid can be effectively controlled by the edge state's dielectric environment. This is reflected in a tunability of the Luttinger parameter K, distinct on different edges of the crystal, and extracted to high accuracy from the statistics of tunnelling spectra at tens of tunnelling points. The interplay of topology and many-body correlations in 1D helical systems has been suggested as a potential avenue towards realising non-Abelian parafermions.

*Phys Chem Chem Phys ; 24(29): 17879-17884, 2022 Jul 27.*

##### RESUMO

We present an in-depth discussion of the magnetic ground state of α''-Fe16N2 within the framework of the density functional theory (DFT). The exchange-correlation effects are treated using a variety of schemes, including the local-spin-density approximation, the generalized-gradient approximation, and the Strongly-Constrained-and-Appropriately-Normed (SCAN) scheme. We also delineate effects of adding an on-site interaction parameter U on the Fe sites. Among all the schemes considered, only SCAN+U is found to capture the surprisingly large magnetization density in α''-Fe16N2 that has been observed experimentally. Our study shows how the combination of SCAN and self-interaction corrections applied on different Fe sites through the parameter U can reproduce both the correct equilibrium volume and the giant magnetization density of α''-Fe16N2.

*Adv Mater ; 34(15): e2108790, 2022 Apr.*

##### RESUMO

Breaking time-reversal symmetry by introducing magnetic order, thereby opening a gap in the topological surface state bands, is essential for realizing useful topological properties such as the quantum anomalous Hall and axion insulator states. In this work, a novel topological antiferromagnetic (AFM) phase is created at the interface of a sputtered, c-axis-oriented, topological insulator/ferromagnet heterostructure-Bi2 Te3 /Ni80 Fe20 because of diffusion of Ni in Bi2 Te3 (Ni-Bi2 Te3 ). The AFM property of the Ni-Bi2 Te3 interfacial layer is established by observation of spontaneous exchange bias in the magnetic hysteresis loop and compensated moments in the depth profile of the magnetization using polarized neutron reflectometry. Analysis of the structural and chemical properties of the Ni-Bi2 Te3 layer is carried out using selected-area electron diffraction, electron energy loss spectroscopy, and X-ray photoelectron spectroscopy. These studies, in parallel with first-principles calculations, indicate a solid-state chemical reaction that leads to the formation of Ni-Te bonds and the presence of topological antiferromagnetic (AFM) compound NiBi2 Te4 in the Ni-Bi2 Te3 interface layer. The Neél temperature of the Ni-Bi2 Te3 layer is ≈63 K, which is higher than that of typical magnetic topological insulators (MTIs). The presented results provide a pathway toward industrial complementary metal-oxide-semiconductor (CMOS)-process-compatible sputtered-MTI heterostructures, leading to novel materials for topological quantum devices.

*Nat Commun ; 13(1): 492, 2022 Jan 25.*

##### RESUMO

Being atomically thin and amenable to external controls, two-dimensional (2D) materials offer a new paradigm for the realization of patterned qubit fabrication and operation at room temperature for quantum information sciences applications. Here we show that the antisite defect in 2D transition metal dichalcogenides (TMDs) can provide a controllable solid-state spin qubit system. Using high-throughput atomistic simulations, we identify several neutral antisite defects in TMDs that lie deep in the bulk band gap and host a paramagnetic triplet ground state. Our in-depth analysis reveals the presence of optical transitions and triplet-singlet intersystem crossing processes for fingerprinting these defect qubits. As an illustrative example, we discuss the initialization and readout principles of an antisite qubit in WS2, which is expected to be stable against interlayer interactions in a multilayer structure for qubit isolation and protection in future qubit-based devices. Our study opens a new pathway for creating scalable, room-temperature spin qubits in 2D TMDs.

*Nature ; 595(7868): 521-525, 2021 07.*

##### RESUMO

Whereas ferromagnets have been known and used for millennia, antiferromagnets were only discovered in the 1930s1. At large scale, because of the absence of global magnetization, antiferromagnets may seem to behave like any non-magnetic material. At the microscopic level, however, the opposite alignment of spins forms a rich internal structure. In topological antiferromagnets, this internal structure leads to the possibility that the property known as the Berry phase can acquire distinct spatial textures2,3. Here we study this possibility in an antiferromagnetic axion insulator-even-layered, two-dimensional MnBi2Te4-in which spatial degrees of freedom correspond to different layers. We observe a type of Hall effect-the layer Hall effect-in which electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under zero electric field, even-layered MnBi2Te4 shows no anomalous Hall effect. However, applying an electric field leads to the emergence of a large, layer-polarized anomalous Hall effect of about 0.5e2/h (where e is the electron charge and h is Planck's constant). This layer Hall effect uncovers an unusual layer-locked Berry curvature, which serves to characterize the axion insulator state. Moreover, we find that the layer-locked Berry curvature can be manipulated by the axion field formed from the dot product of the electric and magnetic field vectors. Our results offer new pathways to detect and manipulate the internal spatial structure of fully compensated topological antiferromagnets4-9. The layer-locked Berry curvature represents a first step towards spatial engineering of the Berry phase through effects such as layer-specific moiré potential.

*Nature ; 594(7862): 213-216, 2021 06.*

##### RESUMO

The electrification of heavy-duty transport and aviation will require new strategies to increase the energy density of electrode materials1,2. The use of anionic redox represents one possible approach to meeting this ambitious target. However, questions remain regarding the validity of the O2-/O- oxygen redox paradigm, and alternative explanations for the origin of the anionic capacity have been proposed3, because the electronic orbitals associated with redox reactions cannot be measured by standard experiments. Here, using high-energy X-ray Compton measurements together with first-principles modelling, we show how the electronic orbital that lies at the heart of the reversible and stable anionic redox activity can be imaged and visualized, and its character and symmetry determined. We find that differential changes in the Compton profile with lithium-ion concentration are sensitive to the phase of the electronic wave function, and carry signatures of electrostatic and covalent bonding effects4. Our study not only provides a picture of the workings of a lithium-rich battery at the atomic scale, but also suggests pathways to improving existing battery materials and designing new ones.

*Sci Adv ; 6(30): eaba4275, 2020 Jul.*

##### RESUMO

Novel magnetic topological materials pave the way for studying the interplay between band topology and magnetism. However, an intrinsically ferromagnetic topological material with only topological bands at the charge neutrality energy has so far remained elusive. Using rational design, we synthesized MnBi8Te13, a natural heterostructure with [MnBi2Te4] and [Bi2Te3] layers. Thermodynamic, transport, and neutron diffraction measurements show that despite the adjacent [MnBi2Te4] being 44.1 Å apart, MnBi8Te13 manifests long-range ferromagnetism below 10.5 K with strong coupling between magnetism and charge carriers. First-principles calculations and angle-resolved photoemission spectroscopy measurements reveal it is an axion insulator with sizable surface hybridization gaps. Our calculations further demonstrate the hybridization gap persists in the two-dimensional limit with a nontrivial Chern number. Therefore, as an intrinsic ferromagnetic axion insulator with clean low-energy band structures, MnBi8Te13 serves as an ideal system to investigate rich emergent phenomena, including the quantized anomalous Hall effect and quantized magnetoelectric effect.

*Sci Rep ; 10(1): 12961, 2020 Jul 31.*

##### RESUMO

The rare-earth monopnictide family is attracting an intense current interest driven by its unusual extreme magnetoresistance (XMR) property and the potential presence of topologically non-trivial surface states. The experimental observation of non-trivial surface states in this family of materials are not ubiquitous. Here, using high-resolution angle-resolved photoemission spectroscopy, magnetotransport, and parallel first-principles modeling, we examine the nature of electronic states in HoSb. Although we find the presence of bulk band gaps at the [Formula: see text] and X-symmetry points of the Brillouin zone, we do not find these gaps to exhibit band inversion so that HoSb does not host a Dirac semimetal state. Our magnetotransport measurements indicate that HoSb can be characterized as a correlated nearly-complete electron-hole-compensated semimetal. Our analysis reveals that the nearly perfect electron-hole compensation could drive the appearance of non-saturating XMR effect in HoSb.

*J Phys Condens Matter ; 2020 Jul 29.*

##### RESUMO

High-energy X-ray diffraction (HE-XRD) experiments combined with an analysisbased on atomic-pair-distribution functions can be an effective tool for probing low-dimensional materials. Here, we show how such an analysis can be used to gain insightinto structural properties of PbTe nanoparticles. We interpret our HE-XRD data using anorthorhombic Pnma phase of PbTe, which is an orthorhombic distortion of the rocksalt phase.Although local crystal geometry can vary substantially with particle size at scales below 10 nm,and for very small nanoparticles the particle size itself influences X-ray diffraction patterns,our study shows that HE-XRD can provide a unique nano-characterization tool for unravelingstructural properties of nanoscale systems.

*Sci Rep ; 10(1): 2776, 2020 Feb 17.*

##### RESUMO

The topological nodal-line semimetal (TNS) is a unique class of materials with a one dimensional line node accompanied by a nearly dispersionless two-dimensional surface state. However, a direct observation of the so called drumhead surface state within current nodal-line materials is still elusive. Here, using high-resolution angle-resolved photoemission spectroscopy (ARPES) along with first-principles calculations, we report the observation of a topological nodal-loop (TNL) in SrAs3, whereas CaAs3 exhibits a topologically trivial state. Our data reveal that surface projections of the bulk nodal-points are connected by clear drumhead surface states in SrAs3. Furthermore, our magneto-transport and magnetization data clearly suggest the presence (absence) of surface states in SrAs3 (CaAs3). Notably, the observed topological states in SrAs3 are well separated from other bands in the vicinity of the Fermi level. RAs3 where R = Ca, Sr, thus, offers a unique opportunity to realize an archetype nodal-loop semimetal and establish a platform for obtaining a deeper understanding of the quantum phase transitions.

*ACS Nano ; 14(3): 2718-2728, 2020 Mar 24.*

##### RESUMO

Proximity effects in superconducting normal (SN) material heterostructures with metals and semiconductors have long been observed and theoretically described in terms of Cooper pair wave functions and Andreev reflections. Whereas the semiconducting N-layer materials in the proximity experiments to date have been doped and tens of nanometers thick, we present here a proximity tunneling study involving a pristine single-layer transition-metal dichalcogenide film of MoS2 placed on top of a Pb thin film. Scanning tunneling microscopy and spectroscopy experiments together with parallel theoretical analysis based on electronic structure calculations and Green's function modeling allow us to unveil a two-step process in which MoS2 first becomes metallic and then is induced into becoming a conventional s-wave Bardeen-Cooper-Schrieffer-type superconductor. The lattice mismatch between the MoS2 overlayer and the Pb substrate is found to give rise to a topographic moiré pattern. Even though the induced gap appears uniform in location, the coherence peak height of the tunneling spectra is modulated spatially into a moiré pattern that is similar to but shifted with respect to the moiré pattern observed in topography. The aforementioned modulation is shown to originate from the atomic-scale structure of the SN interface and the nature of local atomic orbitals that are involved in generating the local pairing potential. Our study indicates that the local modulation of induced superconductivity in MoS2 could be controlled via geometrical tuning, and it thus shows promise toward the integration of monolayer superconductors into next-generation functional electronic devices by exploiting proximity-effect control of quantum phases.