Hidden non-collinear spin-order induced topological surface states.

Rare-earth monopnictides are a family of materials simultaneously displaying complex magnetism, strong electronic correlation, and topological band structure. The recently discovered emergent arc-like surface states in these materials have been attributed to the multi-wave-vector antiferromagnetic order, yet the direct experimental evidence has been elusive. Here we report observation of non-collinear antiferromagnetic order with multiple modulations using spin-polarized scanning tunneling microscopy. Moreover, we discover a hidden spin-rotation transition of single-to-multiple modulations 2 K below the Néel temperature. The hidden transition coincides with the onset of the surface states splitting observed by our angle-resolved photoemission spectroscopy measurements. Single modulation gives rise to a band inversion with induced topological surface states in a local momentum region while the full Brillouin zone carries trivial topological indices, and multiple modulation further splits the surface bands via non-collinear spin tilting, as revealed by our calculations. The direct evidence of the non-collinear spin order in NdSb not only clarifies the mechanism of the emergent topological surface states, but also opens up a new paradigm of control and manipulation of band topology with magnetism.

Atomistic Origin of Diverse Charge Density Wave States in CsV_{3}Sb_{5}.

Kagome metals AV_{3}Sb_{5} (A=K, Rb, or Cs) exhibit intriguing charge density wave (CDW) instabilities, which interplay with superconductivity and band topology. However, despite firm observations, the atomistic origins of the CDW phases, as well as hidden instabilities, remain elusive. Here, we adopt our newly developed symmetry-adapted cluster expansion method to construct a first-principles-based effective Hamiltonian of CsV_{3}Sb_{5}, which not only reproduces the established inverse star of David (ISD) phase, but also predict a series of D_{3h}-n states under mild tensile strains. With such atomistic Hamiltonians, the microscopic origins of different CDW states are revealed as the competition of the second-nearest neighbor V-V pairs versus the first-nearest neighbor V-V and V-Sb couplings. Interestingly, the effective Hamiltonians also reveal the existence of ionic Dzyaloshinskii-Moriya interaction in the high-symmetry phase of CsV_{3}Sb_{5} and drives the formation of noncollinear CDW patterns. Our work thus not only deepens the understanding of the CDW formation in AV_{3}Sb_{5}, but also demonstrates that the effective Hamiltonian is a suitable approach for investigating CDW mechanisms, which can be extended to various CDW systems.

Atomically precise engineering of spin-orbit polarons in a kagome magnetic Weyl semimetal.

Atomically precise defect engineering is essential to manipulate the properties of emerging topological quantum materials for practical quantum applications. However, this remains challenging due to the obstacles in modifying the typically complex crystal lattice with atomic precision. Here, we report the atomically precise engineering of the vacancy-localized spin-orbit polarons in a kagome magnetic Weyl semimetal Co3Sn2S2, using scanning tunneling microscope. We achieve the step-by-step repair of the selected vacancies, leading to the formation of artificial sulfur vacancies with elaborate geometry. We find that that the bound states localized around these vacancies undergo a symmetry dependent energy shift towards Fermi level with increasing vacancy size. As the vacancy size increases, the localized magnetic moments of spin-orbit polarons become tunable and eventually become itinerantly negative due to spin-orbit coupling in the kagome flat band. These findings provide a platform for engineering atomic quantum states in topological quantum materials at the atomic scale.

Competing itinerant and local spin interactions in kagome metal FeGe.

The combination of a geometrically frustrated lattice, and similar energy scales between degrees of freedom endows two-dimensional Kagome metals with a rich array of quantum phases and renders them ideal for studying strong electron correlations and band topology. The Kagome metal, FeGe is a noted example of this, exhibiting A-type collinear antiferromagnetic (AFM) order at TN ≈ 400 K, then establishes a charge density wave (CDW) phase coupled with AFM ordered moment below TCDW ≈ 110 K, and finally forms a c-axis double cone AFM structure around TCanting ≈ 60 K. Here we use neutron scattering to demonstrate the presence of gapless incommensurate spin excitations associated with the double cone AFM structure of FeGe at temperatures well above TCanting and TCDW that merge into gapped commensurate spin waves from the A-type AFM order. Commensurate spin waves follow the Bose factor and fit the Heisenberg Hamiltonian, while the incommensurate spin excitations, emerging below TN where AFM order is commensurate, start to deviate from the Bose factor around TCDW, and peaks at TCanting. This is consistent with a critical scattering of a second order magnetic phase transition with decreasing temperature. By comparing these results with density functional theory calculations, we conclude that the incommensurate magnetic structure arises from the nested Fermi surfaces of itinerant electrons and the formation of a spin density wave order.

Tunable vortex bound states in multiband CsV3Sb5-derived kagome superconductors.

Vortices and bound states offer an effective means of comprehending the electronic properties of superconductors. Recently, surface-dependent vortex core states have been observed in the newly discovered kagome superconductors CsV3Sb5. Although the spatial distribution of the sharp zero energy conductance peak appears similar to Majorana bound states arising from the superconducting Dirac surface states, its origin remains elusive. In this study, we present observations of tunable vortex bound states (VBSs) in two chemically-doped kagome superconductors Cs(V1-xTrx)3Sb5 (Tr = Ta or Ti), using low-temperature scanning tunneling microscopy/spectroscopy. The CsV3Sb5-derived kagome superconductors exhibit full-gap-pairing superconductivity accompanied by the absence of long-range charge orders, in contrast to pristine CsV3Sb5. Zero-energy conductance maps demonstrate a field-driven continuous reorientation transition of the vortex lattice, suggesting multiband superconductivity. The Ta-doped CsV3Sb5 displays the conventional cross-shaped spatial evolution of Caroli-de Gennes-Matricon bound states, while the Ti-doped CsV3Sb5 exhibits a sharp, non-split zero-bias conductance peak (ZBCP) that persists over a long distance across the vortex. The spatial evolution of the non-split ZBCP is robust against surface effects and external magnetic field but is related to the doping concentrations. Our study reveals the tunable VBSs in multiband chemically-doped CsV3Sb5 system and offers fresh insights into previously reported Y-shaped ZBCP in a non-quantum-limit condition at the surface of kagome 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.

De Haas-van Alphen spectroscopy and magnetic breakdown in moiré graphene.

Quantum oscillations originating from the quantization of electron cyclotron orbits provide sensitive diagnostics of electron bands and interactions. We report on nanoscale imaging of the thermodynamic magnetization oscillations caused by the de Haas-van Alphen effect in moiré graphene. Scanning by means of superconducting quantum interference device (SQUID)-on-tip in Bernal bilayer graphene crystal axis-aligned to hexagonal boron nitride reveals large magnetization oscillations with amplitudes reaching 500 Bohr magneton per electron in weak magnetic fields, unexpectedly low frequencies, and high sensitivity to superlattice filling fraction. The oscillations allow us to reconstruct the complex band structure, revealing narrow moiré bands with multiple overlapping Fermi surfaces separated by unusually small momentum gaps. We identified sets of oscillations that violate the textbook Onsager Fermi surface sum rule, signaling formation of broad-band particle-hole superposition states induced by coherent magnetic breakdown.

Unification of Nonlinear Anomalous Hall Effect and Nonreciprocal Magnetoresistance in Metals by the Quantum Geometry.

The quantum geometry has significant consequences in determining transport and optical properties in quantum materials. Here, we use a semiclassical formalism coupled with perturbative corrections unifying the nonlinear anomalous Hall effect and nonreciprocal magnetoresistance (longitudinal resistance) from the quantum geometry. In the dc limit, both transverse and longitudinal nonlinear conductivities include a term due to the normalized quantum metric dipole. The quantum metric contribution is intrinsic and does not scale with the quasiparticle lifetime. We demonstrate the coexistence of a nonlinear anomalous Hall effect and nonreciprocal magnetoresistance in films of the doped antiferromagnetic topological insulator MnBi_{2}Te_{4}. Our work indicates that both longitudinal and transverse nonlinear transport provide a sensitive probe of the quantum geometry in solids.

Observation of interband Berry phase in laser-driven crystals.

Ever since its discovery1, the notion of the Berry phase has permeated all branches of physics and plays an important part in a variety of quantum phenomena2. However, so far all its realizations have been based on a continuous evolution of the quantum state, following a cyclic path. Here we introduce and demonstrate a conceptually new manifestation of the Berry phase in light-driven crystals, in which the electronic wavefunction accumulates a geometric phase during a discrete evolution between different bands, while preserving the coherence of the process. We experimentally reveal this phase by using a strong laser field to engineer an internal interferometer, induced during less than one cycle of the driving field, which maps the phase onto the emission of higher-order harmonics. Our work provides an opportunity for the study of geometric phases, leading to a variety of observations in light-driven topological phenomena and attosecond solid-state physics.

Imaging quantum oscillations and millitesla pseudomagnetic fields in graphene.

The exceptional control of the electronic energy bands in atomically thin quantum materials has led to the discovery of several emergent phenomena1. However, at present there is no versatile method for mapping the local band structure in advanced two-dimensional materials devices in which the active layer is commonly embedded in the insulating layers and metallic gates. Using a scanning superconducting quantum interference device, here we image the de Haas-van Alphen quantum oscillations in a model system, the Bernal-stacked trilayer graphene with dual gates, which shows several highly tunable bands2-4. By resolving thermodynamic quantum oscillations spanning more than 100 Landau levels in low magnetic fields, we reconstruct the band structure and its evolution with the displacement field with excellent precision and nanoscale spatial resolution. Moreover, by developing Landau-level interferometry, we show shear-strain-induced pseudomagnetic fields and map their spatial dependence. In contrast to artificially induced large strain, which leads to pseudomagnetic fields of hundreds of tesla5-7, we detect naturally occurring pseudomagnetic fields as low as 1 mT corresponding to graphene twisting by 1 millidegree, two orders of magnitude lower than the typical angle disorder in twisted bilayer graphene8-11. This ability to resolve the local band structure and strain at the nanoscale level enables the characterization and use of tunable band engineering in practical van der Waals devices.

Monopole-like orbital-momentum locking and the induced orbital transport in topological chiral semimetals.

The interplay between chirality and topology nurtures many exotic electronic properties. For instance, topological chiral semimetals display multifold chiral fermions that manifest nontrivial topological charge and spin texture. They are an ideal playground for exploring chirality-driven exotic physical phenomena. In this work, we reveal a monopole-like orbital-momentum locking texture on the three-dimensional Fermi surfaces of topological chiral semimetals with B20 structures (e.g., RhSi and PdGa). This orbital texture enables a large orbital Hall effect (OHE) and a giant orbital magnetoelectric (OME) effect in the presence of current flow. Different enantiomers exhibit the same OHE which can be converted to the spin Hall effect by spin-orbit coupling in materials. In contrast, the OME effect is chirality-dependent and much larger than its spin counterpart. Our work reveals the crucial role of orbital texture for understanding OHE and OME effects in topological chiral semimetals and paves the path for applications in orbitronics, spintronics, and enantiomer recognition.

First-order quantum phase transition in the hybrid metal-Mott insulator transition metal dichalcogenide 4Hb-TaS2.

Coupling together distinct correlated and topologically nontrivial electronic phases of matter can potentially induce novel electronic orders and phase transitions among them. Transition metal dichalcogenide compounds serve as a bedrock for exploration of such hybrid systems. They host a variety of exotic electronic phases, and their Van der Waals nature enables to admix them, either by exfoliation and stacking or by stoichiometric growth, and thereby induce novel correlated complexes. Here, we investigate the compound 4Hb-TaS2 that interleaves the Mott-insulating state of 1T-TaS2 and the putative spin liquid it hosts together with the metallic state of 2H-TaS2 and the low-temperature superconducting phase it harbors using scanning tunneling spectroscopy. We reveal a thermodynamic phase diagram that hosts a first-order quantum phase transition between a correlated Kondo-like cluster state and a depleted flat band state. We demonstrate that this intrinsic transition can be induced by an electric field and temperature as well as by manipulation of the interlayer coupling with the probe tip, hence allowing to reversibly toggle between the Kondo-like cluster and the depleted flat band states. The phase transition is manifested by a discontinuous change of the complete electronic spectrum accompanied by hysteresis and low-frequency noise. We find that the shape of the transition line in the phase diagram is determined by the local compressibility and the entropy of the two electronic states. Our findings set such heterogeneous structures as an exciting platform for systematic investigation and manipulation of Mott-metal transitions and strongly correlated phases and quantum phase transitions therein.

Chiral Charge Density Wave and Backscattering-Immune Orbital Texture in Monolayer 1T-TiTe2.

Nontrivial electronic states are attracting intense attention in low-dimensional physics. Though chirality has been identified in charge states with a scalar order parameter, its intertwining with charge density waves (CDW), film thickness, and the impact on the electronic behaviors remain less well understood. Here, using scanning tunneling microscopy, we report a 2 × 2 chiral CDW as well as a strong suppression of the Te-5p hole-band backscattering in monolayer 1T-TiTe2. These exotic characters vanish in bilayer TiTe2 in a non-CDW state. Theoretical calculations prove that chirality comes from a helical stacking of the triple-q CDW components and, therefore, can persist at the two-dimensional limit. Furthermore, the chirality renders the Te-5p bands with an unconventional orbital texture that prohibits electron backscattering. Our study establishes TiTe2 as a promising playground for manipulating the chiral ground states at the monolayer limit and provides a novel path to engineer electronic properties from an orbital degree.

Direct observation of the collective modes of the charge density wave in the kagome metal CsV3Sb5.

A recently discovered group of kagome metals AV[Formula: see text]Sb[Formula: see text] (A = K, Rb, Cs) exhibit a variety of intertwined unconventional electronic phases, which emerge from a puzzling charge density wave phase. Understanding of this charge-ordered parent phase is crucial for deciphering the entire phase diagram. However, the mechanism of the charge density wave is still controversial, and its primary source of fluctuations-the collective modes-has not been experimentally observed. Here, we use ultrashort laser pulses to melt the charge order in CsV[Formula: see text]Sb[Formula: see text] and record the resulting dynamics using femtosecond angle-resolved photoemission. We resolve the melting time of the charge order and directly observe its amplitude mode, imposing a fundamental limit for the fastest possible lattice rearrangement time. These observations together with ab initio calculations provide clear evidence for a structural rather than electronic mechanism of the charge density wave. Our findings pave the way for a better understanding of the unconventional phases hosted on the kagome lattice.

Interplay of structural chirality, electron spin and topological orbital in chiral molecular spin valves.

Chirality has been a property of central importance in physics, chemistry and biology for more than a century. Recently, electrons were found to become spin polarized after transmitting through chiral molecules, crystals, and their hybrids. This phenomenon, called chirality-induced spin selectivity (CISS), presents broad application potentials and far-reaching fundamental implications involving intricate interplays among structural chirality, topological states, and electronic spin and orbitals. However, the microscopic picture of how chiral geometry influences electronic spin remains elusive, given the negligible spin-orbit coupling (SOC) in organic molecules. In this work, we address this issue via a direct comparison of magnetoconductance (MC) measurements on magnetic semiconductor-based chiral molecular spin valves with normal metal electrodes of contrasting SOC strengths. The experiment reveals that a heavy-metal electrode provides SOC to convert the orbital polarization induced by the chiral molecular structure to spin polarization. Our results illustrate the essential role of SOC in the metal electrode for the CISS spin valve effect. A tunneling model with a magnetochiral modulation of the potential barrier is shown to quantitatively account for the unusual transport behavior.

Abundant Lattice Instability in Kagome Metal ScV_{6}Sn_{6}.

Kagome materials are emerging platforms for studying charge and spin orders. In this Letter, we have revealed a rich lattice instability in a Z_{2} kagome metal ScV_{6}Sn_{6} by first-principles calculations. Beyond verifying the sqrt[3]×sqrt[3]×3 charge density wave (CDW) order observed by the recent experiment, we further identified three more possible CDW structures, i.e., sqrt[3]×sqrt[3]×2 CDW with P6/mmm symmetry, 2×2×2 CDW with Immm symmetry, and 2×2×2 CDW with P6/mmm symmetry. The former two are more energetically favored than the sqrt[3]×sqrt[3]×3 phase, while the third one is comparable in energy. These CDW distortions involve mainly out-of-plane motions of Sc and Sn atoms, while V atoms constituting the kagome net are almost unchanged. We attribute the lattice instability to the smallness of Sc atomic radius. In contrast, such instability disappears in its sister compounds RV_{6}Sn_{6} (R is Y, or a rare-earth element), which exhibit quite similar electronic band structures to the Sc compound, because R has a larger atomic radius. Our work indicates that ScV_{6}Sn_{6} might exhibit varied CDW phases in different experimental conditions and provides insights to explore rich charge orders in kagome materials.

Quantum-metric-induced nonlinear transport in a topological antiferromagnet.

The Berry curvature and quantum metric are the imaginary part and real part, respectively, of the quantum geometric tensor, which characterizes the topology of quantum states1. The Berry curvature is known to generate a number of important transport phenomena, such as the quantum Hall effect and the anomalous Hall effect2,3; however, the consequences of the quantum metric have rarely been probed by transport measurements. Here we report the observation of quantum-metric-induced nonlinear transport, including both a nonlinear anomalous Hall effect and a diode-like non-reciprocal longitudinal response, in thin films of a topological antiferromagnet, MnBi2Te4. Our observations reveal that the transverse and longitudinal nonlinear conductivities reverse signs when reversing the antiferromagnetic order, diminish above the Néel temperature and are insensitive to disorder scattering, thus verifying their origin in the band-structure topology. They also flip signs between electron- and hole-doped regions, in agreement with theoretical calculations. Our work provides a means to probe the quantum metric through nonlinear transport and to design magnetic nonlinear devices.

Electrical switching of ferro-rotational order in nanometre-thick 1T-TaS2 crystals.

Hysteretic switching of domain states is a salient characteristic of all ferroic materials and the foundation for their multifunctional applications. Ferro-rotational order is emerging as a type of ferroic order that features structural rotations, but control over state switching remains elusive due to its invariance under both time reversal and spatial inversion. Here we demonstrate electrical switching of ferro-rotational domain states in the charge-density-wave phases of nanometre-thick 1T-TaS2 crystals. Cooling from the high-symmetry phase to the ferro-rotational phase under an external electric field induces domain state switching and domain wall formation, which is realized in a simple two-terminal configuration using a volt-scale bias. Although the electric field does not couple with the order due to symmetry mismatch, it drives domain wall propagation to give rise to reversible, durable and non-volatile isothermal state switching at room temperature. These results offer a route to the manipulation of ferro-rotational order and its nanoelectronic applications.

General nonlinear Hall current in magnetic insulators beyond the quantum anomalous Hall effect.

Can a generic magnetic insulator exhibit a Hall current? The quantum anomalous Hall effect (QAHE) is one example of an insulating bulk carrying a quantized Hall conductivity while insulators with zero Chern number present zero Hall conductance in the linear response regime. Here, we find that a general magnetic insulator possesses a nonlinear Hall conductivity quadratic to the electric field if the system breaks inversion symmetry, which can be identified as a new type of multiferroic coupling. This conductivity originates from an induced orbital magnetization due to virtual interband transitions. We identify three contributions to the wavepacket motion, a velocity shift, a positional shift, and a Berry curvature renormalization. In contrast to the crystalline solid, we find that this nonlinear Hall conductivity vanishes for Landau levels of a 2D electron gas, indicating a fundamental difference between the QAHE and the integer quantum Hall effect.

Para-hydrodynamics from weak surface scattering in ultraclean thin flakes.

Electron hydrodynamics typically emerges in electron fluids with a high electron-electron collision rate. However, new experiments with thin flakes of WTe2 have revealed that other momentum-conserving scattering processes can replace the role of the electron-electron interaction, thereby leading to a novel, so-called para-hydrodynamic regime. Here, we develop the kinetic theory for para-hydrodynamic transport. To this end, we consider a ballistic electron gas in a thin three-dimensional sheet where the momentum-relaxing (lmr) and momentum-conserving (lmc) mean free paths are decreased due to boundary scattering from a rough surface. The resulting effective mean free path of the in-plane components of the electronic flow is then expressed in terms of microscopic parameters of the sheet boundaries, predicting that a para-hydrodynamic regime with lmr ≫ lmc emerges generically in ultraclean three-dimensional materials. Using our approach, we recover the transport properties of WTe2 in the para-hydrodynamic regime in good agreement with existing experiments.