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Moiré superlattices formed by van der Waals materials can support a wide range of electronic phases, including Mott insulators1-4, superconductors5-10 and generalized Wigner crystals2. When excitons are confined by a moiré superlattice, a new class of exciton emerges, which holds promise for realizing artificial excitonic crystals and quantum optical effects11-16. When such moiré excitons are coupled to charge carriers, correlated states may arise. However, no experimental evidence exists for charge-coupled moiré exciton states, nor have their properties been predicted by theory. Here we report the optical signatures of trions coupled to the moiré potential in tungsten diselenide/molybdenum diselenide heterobilayers. The moiré trions show multiple sharp emission lines with a complex charge-density dependence, in stark contrast to the behaviour of conventional trions. We infer distinct contributions to the trion emission from radiative decay in which the remaining carrier resides in different moiré minibands. Variation of the trion features is observed in different devices and sample areas, indicating high sensitivity to sample inhomogeneity and variability. The observation of these trion features motivates further theoretical and experimental studies of higher-order electron correlation effects in moiré superlattices.
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Moiré superlattices (MSLs) formed in van der Waals materials have become a promising platform to realize novel two-dimensional electronic states. Angle-aligned trilayer structures can form two sets of MSLs which could potentially interfere. In this work, we directly image the moiré patterns in both monolayer and twisted bilayer graphene aligned on hexagonal boron nitride (hBN), using combined scanning microwave impedance microscopy and conductive atomic force microscopy. Correlation of the two techniques reveals the contrast mechanism for the achieved ultrahigh spatial resolution (<2 nm). We observe two sets of MSLs with different periodicities in the trilayer stack. The smaller MSL breaks the 6-fold rotational symmetry and exhibits abrupt discontinuities at the boundaries of the larger MSL. Using a rigid atomic-stacking model, we demonstrate that the hBN layer considerably modifies the MSL of twisted bilayer graphene. We further analyze its effect on the reciprocal space spectrum of the dual-moiré system.
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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.
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We have measured the reflectance contrast, photoluminescence, and valley polarization of a WSe_{2}/WS_{2} heterobilayer moiré superlattice at gate-tunable charge density. We observe absorption modulation of three intralayer moiré excitons at filling factors ν=1/3 and 2/3. We also observe luminescence modulation of interlayer trions at around a dozen fractional filling factors, including ν=-3/2, 1/4, 1/3, 2/5, 2/3, 6/7, 5/3. Remarkably, the valley polarization of interlayer trions is suppressed at some fractional fillings. These results demonstrate that electron crystallization can modulate the absorption, emission, and valley dynamics of the excitonic states in a moiré superlattice.
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The magnetic properties in two-dimensional van der Waals materials depend sensitively on structure. CrI3, as an example, has been recently demonstrated to exhibit distinct magnetic properties depending on the layer thickness and stacking order. Bulk CrI3 is ferromagnetic (FM) with a Curie temperature of 61 K and a rhombohedral layer stacking, whereas few-layer CrI3 has a layered antiferromagnetic (AFM) phase with a lower ordering temperature of 45 K and a monoclinic stacking. In this work, we use cryogenic magnetic force microscopy to investigate CrI3 flakes in the intermediate thickness range (25-200 nm) and find that the two types of magnetic orders, hence the stacking orders, can coexist in the same flake with a layer of â¼13 nm at each surface being in the layered AFM phase similar to few-layer CrI3 and the rest in the bulk FM phase. The switching of the bulk moment proceeds through a remnant state with nearly compensated magnetic moment along the c-axis, indicating formation of c-axis domains allowed by a weak interlayer coupling strength in the rhombohedral phase. Our results provide a comprehensive picture on the magnetism in CrI3 and point to the possibility of engineering magnetic heterostructures within the same material.
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Two-dimensional ferromagnet Cr2Ge2Te6 (CGT) is so resistive below its Curie temperature that probing its magnetism by electrical transport becomes extremely difficult. By forming heterostructures with Pt, however, we observe clear anomalous Hall effect (AHE) in 5 nm thick Pt deposited on thin (<50 nm) exfoliated flakes of CGT. The AHE hysteresis loops persist to â¼60 K, which matches well to the Curie temperature of CGT obtained from the bulk magnetization measurements. The slanted AHE loops with a narrow opening indicate magnetic domain formation, which is confirmed by low-temperature magnetic force microscopy (MFM) imaging. These results clearly demonstrate that CGT imprints its magnetization in the AHE signal of the Pt layer. Density functional theory calculations of CGT/Pt heterostructures suggest that the induced ferromagnetism in Pt may be primarily responsible for the observed AHE. Our results establish a powerful way of investigating magnetism in 2D insulating ferromagnets, which can potentially work for monolayer devices.
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We report simultaneous transport and scanning microwave impedance microscopy to examine the correlation between transport quantization and filling of the bulk Landau levels in the quantum Hall regime in gated graphene devices. Surprisingly, a comparison of these measurements reveals that quantized transport typically occurs below the complete filling of bulk Landau levels, when the bulk is still conductive. This result points to a revised understanding of transport quantization when carriers are accumulated by gating. We discuss the implications on transport study of the quantum Hall effect in graphene and related topological states in other two-dimensional electron systems.
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This corrects the article DOI: 10.1103/PhysRevLett.115.265701.
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Complex many-body interaction in perovskite manganites gives rise to a strong competition between ferromagnetic metallic and charge-ordered phases with nanoscale electronic inhomogeneity and glassy behaviors. Investigating this glassy state requires high-resolution imaging techniques with sufficient sensitivity and stability. Here, we present the results of a near-field microwave microscope imaging on the strain-driven glassy state in a manganite film. The high contrast between the two electrically distinct phases allows direct visualization of the phase separation. The low-temperature microscopic configurations differ upon cooling with different thermal histories. At sufficiently high temperatures, we observe switching between the two phases in either direction. The dynamic switching, however, stops below the glass transition temperature. Compared with the magnetization data, the phase separation was microscopically frozen, while spin relaxation was found in a short period of time.
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Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe2-WS2-WSe2 trilayer moiré superlattice. The quadrupolar excitons exhibit a quadratic dependence on the electric field, distinctively different from the linear Stark shift of the dipolar excitons in heterobilayers. This quadrupolar exciton stems from the hybridization of WSe2 valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe2 layers share one hole laterally confined in one moiré unit cell. In contrast, the hole occupation probability in each layer can be continuously tuned via an out-of-plane electric field, reaching 100% in the top or bottom WSe2 under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moiré system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions.
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Moiré superlattices of semiconducting transition metal dichalcogenides enable unprecedented spatial control of electron wavefunctions, leading to emerging quantum states. The breaking of translational symmetry further introduces a new degree of freedom: high symmetry moiré sites of energy minima behaving as spatially separated quantum dots. We demonstrate the superposition between two moiré sites by constructing a trilayer WSe2/monolayer WS2 moiré heterojunction. The two moiré sites in the first layer WSe2 interfacing WS2 allow the formation of two different interlayer excitons, with the hole residing in either moiré site of the first layer WSe2 and the electron in the third layer WSe2. An electric field can drive the hybridization of either of the interlayer excitons with the intralayer excitons in the third WSe2 layer, realizing the continuous tuning of interlayer exciton hopping between two moiré sites and a superposition of the two interlayer excitons, distinctively different from the natural trilayer WSe2.
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A pure spin current generated within a nonlocal spin valve can exert a spin-transfer torque on a nanomagnet. This nonlocal torque enables new design schemes for magnetic memory devices that do not require the application of large voltages across tunnel barriers that can suffer electrical breakdown. Here we report a quantitative measurement of this nonlocal spin torque using spin-torque-driven ferromagnetic resonance. Our measurement agrees well with the prediction of an effective circuit model for spin transport. Based on this model, we suggest strategies for optimizing the strength of nonlocal torque.
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A Chern insulator is a two-dimensional material that hosts chiral edge states produced by the combination of topology with time reversal symmetry breaking. Such edge states are perfect one-dimensional conductors, which may exist not only on sample edges, but on any boundary between two materials with distinct topological invariants (or Chern numbers). Engineering of such interfaces is highly desirable due to emerging opportunities of using topological edge states for energy-efficient information transmission. Here, we report a chiral edge-current divider based on Chern insulator junctions formed within the layered topological magnet MnBi2Te4. We find that in a device containing a boundary between regions of different thickness, topological domains with different Chern numbers can coexist. At the domain boundary, a Chern insulator junction forms, where we identify a chiral edge mode along the junction interface. We use this to construct topological circuits in which the chiral edge current can be split, rerouted, or switched off by controlling the Chern numbers of the individual domains. Our results demonstrate MnBi2Te4 as an emerging platform for topological circuits design.
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The interplay between band topology and magnetism can give rise to exotic states of matter. For example, magnetically doped topological insulators can realize a Chern insulator that exhibits quantized Hall resistance at zero magnetic field. While prior works have focused on ferromagnetic systems, little is known about band topology and its manipulation in antiferromagnets. Here, we report that MnBi2Te4 is a rare platform for realizing a canted-antiferromagnetic (cAFM) Chern insulator with electrical control. We show that the Chern insulator state with Chern number C = 1 appears as the AFM to canted-AFM phase transition happens. The Chern insulator state is further confirmed by observing the unusual transition of the C = 1 state in the cAFM phase to the C = 2 orbital quantum Hall states in the magnetic field induced ferromagnetic phase. Near the cAFM-AFM phase boundary, we show that the dissipationless chiral edge transport can be toggled on and off by applying an electric field alone. We attribute this switching effect to the electrical field tuning of the exchange gap alignment between the top and bottom surfaces. Our work paves the way for future studies on topological cAFM spintronics and facilitates the development of proof-of-concept Chern insulator devices.
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Moiré coupling in transition metal dichalcogenides (TMDCs) superlattices introduces flat minibands that enable strong electronic correlation and fascinating correlated states, and it also modifies the strong Coulomb-interaction-driven excitons and gives rise to moiré excitons. Here, we introduce the layer degree of freedom to the WSe2/WS2 moiré superlattice by changing WSe2 from monolayer to bilayer and trilayer. We observe systematic changes of optical spectra of the moiré excitons, which directly confirm the highly interfacial nature of moiré coupling at the WSe2/WS2 interface. In addition, the energy resonances of moiré excitons are strongly modified, with their separation significantly increased in multilayer WSe2/monolayer WS2 moiré superlattice. The additional WSe2 layers also modulate the strong electronic correlation strength, evidenced by the reduced Mott transition temperature with added WSe2 layer(s). The layer dependence of both moiré excitons and correlated electronic states can be well described by our theoretical model. Our study presents a new method to tune the strong electronic correlation and moiré exciton bands in the TMDCs moiré superlattices, ushering in an exciting platform to engineer quantum phenomena stemming from strong correlation and Coulomb interaction.
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Multiple magnetic skyrmion phases add an additional degree of freedom for skyrmion-based ultrahigh-density spin memory devices. Extending the field to 2D van der Waals magnets is a rewarding challenge, where the realizable degree of freedoms (e.g., thickness, twist angle, and electrical gating) and high skyrmion density result in intriguing new properties and enhanced functionality. In this work, a van der Waals interface, formed by two 2D ferromagnets Cr2 Ge2 Te6 and Fe3 GeTe2 with a Curie temperature of ≈65 and ≈205 K, respectively, hosting two groups of magnetic skyrmions, is reported. Two sets of topological Hall effect signals are observed below 6s0 K when Cr2 Ge2 Te6 is magnetically ordered. These two groups of skyrmions are directly imaged using magnetic force microscopy, and supported by micromagnetic simulations. Interestingly, the magnetic skyrmions persist in the heterostructure with zero applied magnetic field. The results are promising for the realization of skyrmionic devices based on van der Waals heterostructures hosting multiple skyrmion phases.
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Van der Waals heterostructures offer great versatility to tailor unique interactions at the atomically flat interfaces between dissimilar layered materials and induce novel physical phenomena. By bringing monolayer 1 T' WTe2, a two-dimensional quantum spin Hall insulator, and few-layer Cr2Ge2Te6, an insulating ferromagnet, into close proximity in an heterostructure, we introduce a ferromagnetic order in the former via the interfacial exchange interaction. The ferromagnetism in WTe2 manifests in the anomalous Nernst effect, anomalous Hall effect as well as anisotropic magnetoresistance effect. Using local electrodes, we identify separate transport contributions from the metallic edge and insulating bulk. When driven by an AC current, the second harmonic voltage responses closely resemble the anomalous Nernst responses to AC temperature gradient generated by nonlocal heater, which appear as nonreciprocal signals with respect to the induced magnetization orientation. Our results from different electrodes reveal spin-polarized edge states in the magnetized quantum spin Hall insulator.
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Heterobilayers of transition metal dichalcogenides (TMDCs) can form a moiré superlattice with flat minibands, which enables strong electron interaction and leads to various fascinating correlated states. These heterobilayers also host interlayer excitons in a type-II band alignment, in which optically excited electrons and holes reside on different layers but remain bound by the Coulomb interaction. Here we explore the unique setting of interlayer excitons interacting with strongly correlated electrons, and we show that the photoluminescence (PL) of interlayer excitons sensitively signals the onset of various correlated insulating states as the band filling is varied. When the system is in one of such states, the PL of interlayer excitons is relatively amplified at increased optical excitation power due to reduced mobility, and the valley polarization of interlayer excitons is enhanced. The moiré superlattice of the TMDC heterobilayer presents an exciting platform to engineer interlayer excitons through the periodic correlated electron states.
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The tetra-nuclear copper(II) title complex, [Cu(4)Cl(2)(OH)(4)(C(10)H(8)N(2))(4)](NO(3))(2)·6H(2)O, has a crystallographically imposed centre of symmetry. The metal atoms display a distorted tetragonal-pyramidal coordination geometry, and are linked by two µ(2)- and two µ(3)-hydroxo groups, assuming a chair-like conformation for the Cu(4)O(2) core. In the crystal, the complex mol-ecules are linked into a three-dimensional network by inter-molecular O-Hâ¯O, O-Hâ¯Cl, C-Hâ¯O and C-Hâ¯Cl hydrogen bonds and π-π stacking inter-actions with centroid-centroid separations of 3.724â (2) and 3.767â (3)â Å.
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In the title compound, C(12)H(10)ClN(2) (+)·I(-), the aromatic rings are oriented at a dihedral angle of 54.55â (3)°. In the crystal structure, inter-molecular C-Hâ¯I and C-Hâ¯Cl hydrogen bonds link the mol-ecules.