Light-induced ferromagnetism in moiré superlattices.

Many-body interactions between carriers lie at the heart of correlated physics. The ability to tune such interactions would allow the possibility to access and control complex electronic phase diagrams. Recently, two-dimensional moiré superlattices have emerged as a promising platform for quantum engineering such phenomena1-3. The power of the moiré system lies in the high tunability of its physical parameters by adjusting the layer twist angle1-3, electrical field4-6, moiré carrier filling7-11 and interlayer coupling12. Here we report that optical excitation can highly tune the spin-spin interactions between moiré-trapped carriers, resulting in ferromagnetic order in WS2 /WSe2 moiré superlattices. Near the filling factor of -1/3 (that is, one hole per three moiré unit cells), as the excitation power at the exciton resonance increases, a well-developed hysteresis loop emerges in the reflective magnetic circular dichroism signal as a function of magnetic field, a hallmark of ferromagnetism. The hysteresis loop persists down to charge neutrality, and its shape evolves as the moiré superlattice is gradually filled, indicating changes of magnetic ground state properties. The observed phenomenon points to a mechanism in which itinerant photoexcited excitons mediate exchange coupling between moiré-trapped holes. This exciton-mediated interaction can be of longer range than direct coupling between moiré-trapped holes9, and thus magnetic order arises even in the dilute hole regime. This discovery adds a dynamic tuning knob to the rich many-body Hamiltonian of moiré quantum matter13-19.

Dynamically tunable moiré exciton Rydberg states in a monolayer semiconductor on twisted bilayer graphene.

Moiré excitons are emergent optical excitations in two-dimensional semiconductors with moiré superlattice potentials. Although these excitations have been observed on several platforms, a system with dynamically tunable moiré potential to tailor their properties is yet to be realized. Here we present a continuously tunable moiré potential in monolayer WSe2, enabled by its proximity to twisted bilayer graphene (TBG) near the magic angle. By tuning local charge density via gating, TBG provides a spatially varying and dynamically tunable dielectric superlattice for modulation of monolayer WSe2 exciton wave functions. We observed emergent moiré exciton Rydberg branches with increased energy splitting following doping of TBG due to exciton wave function hybridization between bright and dark Rydberg states. In addition, emergent Rydberg states can probe strongly correlated states in TBG at the magic angle. Our study provides a new platform for engineering moiré excitons and optical accessibility to electronic states with small correlation gaps in TBG.

Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers.

The formation of moiré patterns in crystalline solids can be used to manipulate their electronic properties, which are fundamentally influenced by periodic potential landscapes. In two-dimensional materials, a moiré pattern with a superlattice potential can be formed by vertically stacking two layered materials with a twist and/or a difference in lattice constant. This approach has led to electronic phenomena including the fractal quantum Hall effect1-3, tunable Mott insulators4,5 and unconventional superconductivity6. In addition, theory predicts that notable effects on optical excitations could result from a moiré potential in two-dimensional valley semiconductors7-9, but these signatures have not been detected experimentally. Here we report experimental evidence of interlayer valley excitons trapped in a moiré potential in molybdenum diselenide (MoSe2)/tungsten diselenide (WSe2) heterobilayers. At low temperatures, we observe photoluminescence close to the free interlayer exciton energy but with linewidths over one hundred times narrower (around 100 microelectronvolts). The emitter g-factors are homogeneous across the same sample and take only two values, -15.9 and 6.7, in samples with approximate twist angles of 60 degrees and 0 degrees, respectively. The g-factors match those of the free interlayer exciton, which is determined by one of two possible valley-pairing configurations. At twist angles of approximately 20 degrees the emitters become two orders of magnitude dimmer; however, they possess the same g-factor as the heterobilayer at a twist angle of approximately 60 degrees. This is consistent with the umklapp recombination of interlayer excitons near the commensurate 21.8-degree twist angle7. The emitters exhibit strong circular polarization of the same helicity for a given twist angle, which suggests that the trapping potential retains three-fold rotational symmetry. Together with a characteristic dependence on power and excitation energy, these results suggest that the origin of the observed effects is interlayer excitons trapped in a smooth moiré potential with inherited valley-contrasting physics. This work presents opportunities to control two-dimensional moiré optics through variation of the twist angle.

Visualizing the interplay of Dirac mass gap and magnetism at nanoscale in intrinsic magnetic topological insulators.

In intrinsic magnetic topological insulators, Dirac surface-state gaps are prerequisites for quantum anomalous Hall and axion insulating states. Unambiguous experimental identification of these gaps has proved to be a challenge, however. Here, we use molecular beam epitaxy to grow intrinsic MnBi2Te4 thin films. Using scanning tunneling microscopy/spectroscopy, we directly visualize the Dirac mass gap and its disappearance below and above the magnetic order temperature. We further reveal the interplay of Dirac mass gaps and local magnetic defects. We find that, in high defect regions, the Dirac mass gap collapses. Ab initio and coupled Dirac cone model calculations provide insight into the microscopic origin of the correlation between defect density and spatial gap variations. This work provides unambiguous identification of the Dirac mass gap in MnBi2Te4 and, by revealing the microscopic origin of its gap variation, establishes a material design principle for realizing exotic states in intrinsic magnetic topological insulators.

Discrete scale invariance of the quasi-bound states at atomic vacancies in a topological material.

Recently, log-periodic quantum oscillations have been detected in the topological materials zirconium pentatelluride (ZrTe5) and hafnium pentatelluride (HfTe5), displaying an intriguing discrete scale invariance (DSI) characteristic. In condensed materials, the DSI is considered to be related to the quasi-bound states formed by massless Dirac fermions with strong Coulomb attraction, offering a feasible platform to study the long-pursued atomic-collapse phenomenon. Here, we demonstrate that a variety of atomic vacancies in the topological material HfTe5 can host the geometric quasi-bound states with a DSI feature, resembling an artificial supercritical atom collapse. The density of states of these quasi-bound states is enhanced, and the quasi-bound states are spatially distributed in the "orbitals" surrounding the vacancy sites, which are detected and visualized by low-temperature scanning tunneling microscope/spectroscopy. By applying the perpendicular magnetic fields, the quasi-bound states at lower energies become wider and eventually invisible; meanwhile, the energies of quasi-bound states move gradually toward the Fermi energy (EF). These features are consistent with the theoretical prediction of a magnetic field-induced transition from supercritical to subcritical states. The direct observation of geometric quasi-bound states sheds light on the deep understanding of the DSI in quantum materials.

Even-Odd Layer-Dependent Exchange Bias Effect in MnBi2Te4 Chern Insulator Devices.

Magnetic topological materials with coexisting magnetism and nontrivial band structures exhibit many novel quantum phenomena, including the quantum anomalous Hall effect, the axion insulator state, and the Weyl semimetal phase. As a stoichiometric layered antiferromagnetic topological insulator, thin films of MnBi2Te4 show fascinating even-odd layer-dependent physics. In this work, we fabricate a series of thin-flake MnBi2Te4 devices using stencil masks and observe the Chern insulator state at high magnetic fields. Upon magnetic field training, a large exchange bias effect is observed in odd but not in even septuple layer (SL) devices. Through theoretical calculations, we attribute the even-odd layer-dependent exchange bias effect to the contrasting surface and bulk magnetic properties of MnBi2Te4 devices. Our findings reveal the microscopic magnetic configuration of MnBi2Te4 thin flakes and highlight the challenges in replicating the zero magnetic field quantum anomalous Hall effect in odd SL MnBi2Te4 devices.

Intercell moiré exciton complexes in electron lattices.

Excitons, Coulomb-bound electron-hole pairs, play a crucial role in both optical excitation and correlated phenomena in solids. When excitons interact with other quasiparticles, few- and many-body excited states can appear. Here we report an interaction between exciton and charges enabled by unusual quantum confinement in two-dimensional moiré superlattices, which results in many-body ground states composed of moiré excitons and correlated electron lattices. In an H-stacked (60o-twisted) WS2/WSe2 heterobilayer, we found an interlayer moiré exciton whose hole is surrounded by its partner electron's wavefunction distributed among three adjacent moiré traps. This three-dimensional excitonic structure enables large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the quadrupole facilitates the binding of interlayer moiré excitons to the charges in neighbouring moiré cells, forming intercell charged exciton complexes. Our work provides a framework for understanding and engineering emergent exciton many-body states in correlated moiré charge orders.

Ferroelectric switching of a two-dimensional metal.

A ferroelectric is a material with a polar structure whose polarity can be reversed (switched) by applying an electric field1,2. In metals, itinerant electrons screen electrostatic forces between ions, which explains in part why polar metals are very rare3-7. Screening also excludes external electric fields, apparently ruling out the possibility of ferroelectric switching. However, in principle, a thin enough polar metal could be sufficiently penetrated by an electric field to have its polarity switched. Here we show that the topological semimetal WTe2 provides an embodiment of this principle. Although monolayer WTe2 is centro-symmetric and thus non-polar, the stacked bulk structure is polar. We find that two- or three-layer WTe2 exhibits spontaneous out-of-plane electric polarization that can be switched using gate electrodes. We directly detect and quantify the polarization using graphene as an electric-field sensor8. Moreover, the polarization states can be differentiated by conductivity and the carrier density can be varied to modify the properties. The temperature at which polarization vanishes is above 350 kelvin, and even when WTe2 is sandwiched between graphene layers it retains its switching capability at room temperature, demonstrating a robustness suitable for applications in combination with other two-dimensional materials9-12.

Atomic-Scale Andreev Probe of Unconventional Superconductivity.

Recent emergence of low-dimensional unconventional superconductors and their exotic interface properties calls for new approaches to probe the pairing symmetry, a fundamental and frequently elusive property of the superconducting condensate. Here, we introduce the unique capability of tunneling Andreev reflection (TAR) to probe unconventional pairing symmetry, utilizing the sensitivity of this technique to specific Andreev reflections. Specifically, suppression of the lowest-order Andreev reflection due to quantum interference but emergence of the higher-order Andreev processes provides direct evidence of the sign-changing order parameter in the paradigmatic FeSe superconductor. TAR spectroscopy also reveals two superconducting gaps, points to a possibility of a nodal gap structure, and directly confirms that superconductivity is locally suppressed along the nematic twin boundary, with preferential and near-complete suppression of the larger energy gap. Our findings therefore enable new, atomic-scale insight into microscopic, inhomogeneous, and interfacial properties of emerging quantum materials.

Current-Phase Relation of a WTe2 Josephson Junction.

When a topological insulator is incorporated into a Josephson junction, the system is predicted to reveal the fractional Josephson effect with a 4π-periodic current-phase relation. Here, we report the measurement of a 4π-periodic switching current through an asymmetric SQUID, formed by the higher-order topological insulator WTe2. Contrary to the established opinion, we show that a high asymmetry in critical current and negligible loop inductance are not sufficient by themselves to reliably measure the current-phase relation. Instead, we find that our measurement is heavily influenced by additional inductances originating from the self-formed PdTex inside the junction. We therefore develop a method to numerically recover the current-phase relation of the system and find the 1.5 µm long junction to be best described in the short ballistic limit. Our results highlight the complexity of subtle inductance effects that can give rise to misleading topological signatures in transport measurements.

Nematically Templated Vortex Lattices in Superconducting FeSe.

New pathways to controlling the morphology of superconducting vortex lattices─and their subsequent dynamics─are required to guide and scale vortex world-lines into a computing platform. We have found that the nematic twin boundaries align superconducting vortices in the adjacent terraces due to the incommensurate potential between vortices surrounding twin boundaries and those trapped within them. With the varying density and morphology of twin boundaries, the vortex lattice assumes several distinct structural phases, including square, regular, and irregular one-dimensional lattices. Through concomitant analysis of vortex lattice models, we have inferred the characteristic energetics of the twin boundary potential and furthermore predicted the existence of geometric size effects as a function of increasing confinement by the twin boundaries. These findings extend the ideas of directed control over vortex lattices to intrinsic topological defects and their self-organized networks, which have direct implications for the future design and control of strain-based topological quantum computing architectures.

Polaritonic Probe of an Emergent 2D Dipole Interface.

The use of work-function-mediated charge transfer has recently emerged as a reliable route toward nanoscale electrostatic control of individual atomic layers. Using α-RuCl3 as a 2D electron acceptor, we are able to induce emergent nano-optical behavior in hexagonal boron nitride (hBN) that arises due to interlayer charge polarization. Using scattering-type scanning near-field optical microscopy (s-SNOM), we find that a thin layer of α-RuCl3 adjacent to an hBN slab reduces the propagation length of hBN phonon polaritons (PhPs) in significant excess of what can be attributed to intrinsic optical losses. Concomitant nano-optical spectroscopy experiments reveal a novel resonance that aligns energetically with the region of excess PhP losses. These experimental observations are elucidated by first-principles density-functional theory and near-field model calculations, which show that the formation of a large interfacial dipole suppresses out-of-plane PhP propagation. Our results demonstrate the potential utility of charge-transfer heterostructures for tailoring optoelectronic properties of 2D insulators.

Deterministic switching of a perpendicularly polarized magnet using unconventional spin-orbit torques in WTe2.

Spin-orbit torque (SOT)-driven deterministic control of the magnetic state of a ferromagnet with perpendicular magnetic anisotropy is key to next-generation spintronic applications including non-volatile, ultrafast and energy-efficient data-storage devices. However, field-free deterministic switching of perpendicular magnetization remains a challenge because it requires an out-of-plane antidamping torque, which is not allowed in conventional spin-source materials such as heavy metals and topological insulators due to the system's symmetry. The exploitation of low-crystal symmetries in emergent quantum materials offers a unique approach to achieve SOTs with unconventional forms. Here we report an experimental realization of field-free deterministic magnetic switching of a perpendicularly polarized van der Waals magnet employing an out-of-plane antidamping SOT generated in layered WTe2, a quantum material with a low-symmetry crystal structure. Our numerical simulations suggest that the out-of-plane antidamping torque in WTe2 is essential to explain the observed magnetization switching.

Anomalous Second Harmonic Generation from Atomically Thin MnBi2Te4.

MnBi2Te4 is a van der Waals topological insulator with intrinsic intralayer ferromagnetic exchange and A-type antiferromagnetic interlayer coupling. Theoretically, it belongs to a class of structurally centrosymmetric crystals whose layered antiferromagnetic order breaks inversion symmetry for even layer numbers, making optical second harmonic generation (SHG) an ideal probe of the coupling between the crystal and magnetic structures. Here, we perform magnetic field and temperature-dependent SHG measurements on MnBi2Te4 flakes ranging from bulk to monolayer thickness. We find that the dominant SHG signal from MnBi2Te4 is unexpectedly unrelated to both magnetic state and layer number. We suggest that surface SHG is the likely source of the observed strong SHG, whose symmetry matches that of the MnBi2Te4-vacuum interface. Our results highlight the importance of considering the surface contribution to inversion symmetry-breaking in van der Waals centrosymmetric magnets.

Quantum Spin Hall Edge States and Interlayer Coupling in Twisted Bilayer WTe2.

The quantum spin Hall (QSH) effect, characterized by topologically protected spin-polarized edge states, was recently demonstrated in monolayers of the transition metal dichalcogenide (TMD) WTe2. However, the robustness of this topological protection remains largely unexplored in van der Waals heterostructures containing one or more layers of a QSH insulator. In this work, we use scanning tunneling microscopy and spectroscopy (STM/STS) to explore the topological nature of twisted bilayer (tBL) WTe2. At the tBL edges, we observe the characteristic spectroscopic signatures of the QSH edge states. For small twist angles, a rectangular moiré pattern develops, which results in local modifications of the band structure. Using first-principles calculations, we quantify the interactions in tBL WTe2 and its topological edge states as a function of interlayer distance and conclude that it is possible to engineer the topology of WTe2 bilayers via the twist angle as well as interlayer interactions.

Nanometer-Scale Lateral p-n Junctions in Graphene/α-RuCl3 Heterostructures.

The ability to create nanometer-scale lateral p-n junctions is essential for the next generation of two-dimensional (2D) devices. Using the charge-transfer heterostructure graphene/α-RuCl3, we realize nanoscale lateral p-n junctions in the vicinity of graphene nanobubbles. Our multipronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy (s-SNOM) to simultaneously probe the electronic and optical responses of nanobubble p-n junctions. Our STM/STS results reveal that p-n junctions with a band offset of ∼0.6 eV can be achieved with widths of ∼3 nm, giving rise to electric fields of order 108 V/m. Concurrent s-SNOM measurements validate a point-scatterer formalism for modeling the interaction of surface plasmon polaritons (SPPs) with nanobubbles. Ab initio density functional theory (DFT) calculations corroborate our experimental data and reveal the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for generating p-n nanojunctions in 2D materials.

Hidden Local Symmetry Breaking in a Kagome-Lattice Magnetic Weyl Semimetal.

Exploring the relationship between intriguing physical properties and structural complexity is a central topic in studying modern functional materials. Co3Sn2S2, a newly discovered kagome-lattice magnetic Weyl semimetal, has triggered intense interest owing to the intimate coupling between topological semimetallic states and peculiar magnetic properties. However, the origins of the magnetic phase separation and spin glass state below TC in this ordered compound are two unresolved yet important puzzles in understanding its magnetism. Here, we report the discovery of local symmetry breaking surprisingly co-emerges with the onset of ferromagnetic order in Co3Sn2S2, by a combined use of neutron total scattering and half-polarized neutron diffraction. An anisotropic distortion of the cobalt kagome lattice at the atomic/nano level is also found, with distinct distortion directions among the two Co1 and four Co2 atoms. The mismatch of local and average symmetries occurs below TC, indicating that Co3Sn2S2 evolves to an intrinsically lattice disordered system when the ferromagnetic order is established. The local symmetry breaking with intrinsic lattice disorder provides new understanding of the puzzling magnetic properties. Our density functional theory (DFT) calculation indicates that the local symmetry breaking is expected to reorient local ferromagnetic moments, unveiling the existence of the ferromagnetic instability associated with the lattice instability. Furthermore, DFT calculation unveils that the local symmetry breaking could affect the Weyl property by breaking the mirror plane. Our findings highlight the fundamentally important role that the local symmetry breaking plays in advancing our understanding on the magnetic and topological properties in Co3Sn2S2, which may draw attention to explore the overlooked local symmetry breaking in Co3Sn2S2, its derivatives and more broadly in other topological Dirac/Weyl semimetals and kagome-lattice magnets.

Direct Visualization of Surface Spin-Flip Transition in MnBi_{4}Te_{7}.

We report direct visualization of spin-flip transition of the surface layer in antiferromagnet MnBi_{4}Te_{7}, a natural superlattice of alternating MnBi_{2}Te_{4} and Bi_{2}Te_{3} layers, using cryogenic magnetic force microscopy (MFM). The observation of magnetic contrast across domain walls and step edges confirms that the antiferromagnetic order persists to the surface layers. The magnetic field dependence of the MFM images reveals that the surface magnetic layer undergoes a first-order spin-flip transition at a magnetic field that is lower than the bulk transition, in excellent agreement with a revised Mills model. Our analysis suggests no reduction of the order parameter in the surface magnetic layer, implying robust ferromagnetism in the single-layer limit. The direct visualization of surface spin-flip transition not only opens up exploration of surface metamagnetic transitions in layered antiferromagnets, but also provides experimental support for realizing quantized transport in ultrathin films of MnBi_{4}Te_{7} and other natural superlattice topological magnets.

Electron-Phonon and Spin-Lattice Coupling in Atomically Thin Layers of MnBi2Te4.

MnBi2Te4 represents a new class of magnetic topological insulators in which novel quantum phases emerge at temperatures higher than those found in magnetically doped thin films. Here, we investigate how couplings between electron, spin, and lattice are manifested in the phonon spectra of few-septuple-layer thick MnBi2Te4. After categorizing phonon modes by their symmetries, we study the systematic changes in frequency, line width, and line shape of a spectrally isolated A1g mode. The electron-phonon coupling increases in thinner flakes as manifested in a broader phonon line width, which is likely due to changes of the electron density of states. In 4- and 5-septuple thick samples, the onset of magnetic order below the Néel temperature is concurrent with a transition to an insulating state. We observe signatures of a reduced electron-phonon scattering across this transition as reflected in the reduced Fano parameter. Finally, spin-lattice coupling is measured and modeled from temperature-dependent phonon frequency.

Intertwined Topological and Magnetic Orders in Atomically Thin Chern Insulator MnBi2Te4.

MnBi2Te4, a van der Waals magnet, is an emergent platform for exploring Chern insulator physics. Its layered antiferromagnetic order was predicted to enable even-odd layer number dependent topological states. Furthermore, it becomes a Chern insulator when all spins are aligned by an applied magnetic field. However, the evolution of the bulk electronic structure as the magnetic state is continuously tuned and its dependence on layer number remains unexplored. Here, employing multimodal probes, we establish one-to-one correspondence between bulk electronic structure, magnetic state, topological order, and layer thickness in atomically thin MnBi2Te4 devices. As the magnetic state is tuned through the canted magnetic phase, we observe a band crossing, i.e., the closing and reopening of the bulk band gap, corresponding to the concurrent topological phase transition in both even- and odd-layer-number devices. Our findings shed new light on the interplay between band topology and magnetic order in this newly discovered topological magnet.