Nanoscale Visualization of Symmetry-Breaking Electronic Orders and Magnetic Anisotropy in a Kagome Magnet YMn6Sn6.

A kagome lattice hosts a plethora of quantum states arising from the interplay between nontrivial topology and electron correlations. The recently discovered kagome magnet RMn6Sn6 (R represents a rare-earth element) is believed to showcase a kagome band closely resembling textbook characteristics. Here, we report the characterization of local electronic states and their magnetization response in YMn6Sn6 via scanning tunneling microscopy measurements under vector magnetic fields. Our spectroscopic maps reveal a spontaneously trimerized kagome electronic order in YMn6Sn6, where the 6-fold rotational symmetry is disrupted while translational symmetry is maintained. Further application of an external magnetic field demonstrates a strong coupling of the YMn6Sn6 kagome band to the field, which exhibits an energy shift discrepancy under different field directions, implying the existence of magnetization-response anisotropy and anomalous g factors. Our findings establish YMn6Sn6 as an ideal platform for investigating kagome-derived orbital magnetic moment and correlated magnetic topological states.

Manipulation of Moiré Superlattice in Twisted Monolayer-multilayer Graphene by Moving Nanobubbles.

In the heterostructure of two-dimensional (2D) materials, many novel physics phenomena are strongly dependent on the Moiré superlattice. How to achieve the continuous manipulation of the Moiré superlattice in the same sample is very important to study the evolution of various physical properties. Here, in minimally twisted monolayer-multilayer graphene, we found that bubble-induced strain has a huge impact on the Moiré superlattice. By employing the AFM tip to dynamically and continuously move the nanobubble, we realized the modulation of the Moiré superlattice, like the evolution of regular triangular domains into long strip domain structures with single or double domain walls. We also achieved controllable modulation of the Moiré superlattice by moving multiple nanobubbles and establishing the coupling of nanobubbles. Our work presents a flexible method for continuous and controllable manipulation of Moiré superlattices, which will be widely used to study novel physical properties in 2D heterostructures.

Temperature-Driven Rotation Symmetry-Breaking States in an Atomic Kagome Metal KV3Sb5.

Kagome lattice AV3Sb5 has attracted tremendous interest because it hosts correlated and topological physics. However, an in-depth understanding of the temperature-driven electronic states in AV3Sb5 is elusive. Here we use scanning tunneling microscopy to directly capture the rotational symmetry-breaking effect in KV3Sb5. Through both topography and spectroscopic imaging of defect-free KV3Sb5, we observe a charge density wave (CDW) phase transition from an a0 × a0 atomic lattice to a robust 2a0 × 2a0 superlattice upon cooling the sample to 60 K. An individual Sb-atom vacancy in KV3Sb5 further gives rise to the local Friedel oscillation (FO), visible as periodic charge modulations in spectroscopic maps. The rotational symmetry of the FO tends to break at the temperature lower than 40 K. Moreover, the FO intensity shows an obvious competition against the intensity of the CDW. Our results reveal a tantalizing electronic nematicity in KV3Sb5, highlighting the multiorbital correlation in the kagome lattice framework.

Selective Formation of Homochiral Dimers by Intermolecular Charge Transfer on a hBN Nanomesh.

In this study, a comprehensive characterization was conducted on a chiral starburst molecule (C57H48N4, SBM) using scanning tunneling microscopy. When adsorbed onto the hBN/Rh(111) nanomesh, these molecules demonstrate homochiral recognition, leading to a selective formation of homochiral dimers. Further tip manipulation experiments reveal that the chiral dimers are stable and primarily controlled by strong intermolecular interactions. Density functional theory (DFT) calculations supported that the chiral recognition of SBM molecules is governed by the intermolecular charge transfer mechanism, different from the common steric hindrance effect. This study emphasizes the importance of intermolecular charge transfer interactions, offering valuable insights into the chiral recognition of a simple bimolecular system. These findings hold significance for the future advancement in chirality-based electronic sensors and pharmaceuticals, where the chirality of molecules can impact their properties.

Optoelectronically navigated nano-kirigami microrotors.

With the rapid development of micro/nanofabrication technologies, the concept of transformable kirigami has been applied for device fabrication in the microscopic world. However, most nano-kirigami structures and devices were typically fabricated or transformed at fixed positions and restricted to limited mechanical motion along a single axis due to their small sizes, which significantly limits their functionalities and applications. Here, we demonstrate the precise shaping and position control of nano-kirigami microrotors. Metallic microrotors with size of ~10 micrometers were deliberately released from the substrates and readily manipulated through the multimode actuation with controllable speed and direction using an advanced optoelectronic tweezers technique. The underlying mechanisms of versatile interactions between the microrotors and electric field are uncovered by theoretical modeling and systematic analysis. This work reports a novel methodology to fabricate and manipulate micro/nanorotors with well-designed and sophisticated kirigami morphologies, providing new solutions for future advanced optoelectronic micro/nanomachinery.

Formation of Si nanopillars through partial sacrificing in super passivation reactive ion etching.

The vertical gate-all-around (VGAA) metal-oxide-semiconductor field-effect transistor (MOSFET) holds remarkable potential in the three-dimensional (3D) integrated circuits (ICs), primarily owing to its capacity for vertical integration. The Si nanopillar, a crucial channel in the VGAA MOSFET, is conventionally shaped via the reactive ion etching (RIE) system employing SF6/O2. Past studies have indicated that high O2gas conditions in RIE often result in Si grasses irregular nanostructures, such as nanospikes on the bottom surface, due to over-passivation. However, this study revealed that ultrahigh O2proportions (>70%), especially when combined with low chamber pressure, inhibit the development of Si grasses in the RIE system (termed as super passivation). Nevertheless, this scenario leads to the segmentation of the Si nanopillar. To address this issue, a proposed partial sacrificing method, achieved by sacrificing the upper segment of the nanopillar through prolonged processing time and reduced mask size, successfully yielded Si nanopillars without Si grasses. Furthermore, an empirical model was developed to elucidate how experimental parameters influence etching characteristics, encompassing etching rate and Si nanopillar shape, through a systematic examination of the RIE etching process. This research significantly contributes to the production of VGAA MOSFETs and 3D ICs.

Quantum spin liquid signatures in monolayer 1T-NbSe2.

Quantum spin liquids (QSLs) are in a quantum disordered state that is highly entangled and has fractional excitations. As a highly sought-after state of matter, QSLs were predicted to host spinon excitations and to arise in frustrated spin systems with large quantum fluctuations. Here we report on the experimental observation and theoretical modeling of QSL signatures in monolayer 1T-NbSe2, which is a newly emerging two-dimensional material that exhibits both charge-density-wave (CDW) and correlated insulating behaviors. By using scanning tunneling microscopy and spectroscopy (STM/STS), we confirm the presence of spin fluctuations in monolayer 1T-NbSe2 by observing the Kondo resonance as monolayer 1T-NbSe2 interacts with metallic monolayer 1H-NbSe2. Subsequent STM/STS imaging of monolayer 1T-NbSe2 at the Hubbard band energy further reveals a long-wavelength charge modulation, in agreement with the spinon modulation expected for QSLs. By depositing manganese-phthalocyanine (MnPc) molecules with spin S = 3/2 onto monolayer 1T-NbSe2, new STS resonance peaks emerge at the Hubbard band edges of monolayer 1T-NbSe2. This observation is consistent with the spinon Kondo effect induced by a S = 3/2 magnetic impurity embedded in a QSL. Taken together, these experimental observations indicate that monolayer 1T-NbSe2 is a new promising QSL material.

Visualization of Confined Electrons at Grain Boundaries in a Monolayer Charge-Density-Wave Metal.

1D grain boundaries in transition metal dichalcogenides (TMDs) are ideal for investigating the collective electron behavior in confined systems. However, clear identification of atomic structures at the grain boundaries, as well as precise characterization of the electronic ground states, have largely been elusive. Here, direct evidence for the confined electronic states and the charge density modulations at mirror twin boundaries (MTBs) of monolayer NbSe2 , a representative charge-density-wave (CDW) metal, is provided. The scanning tunneling microscopy (STM) measurements, accompanied by the first-principles calculations, reveal that there are two types of MTBs in monolayer NbSe2 , both of which exhibit band bending effect and 1D boundary states. Moreover, the intrinsic CDW signatures of monolayer NbSe2 are dramatically suppressed as approaching an isolated MTB but can be either enhanced or suppressed in the MTB-constituted confined wedges. Such a phenomenon can be well explained by the MTB-CDW interference interactions. The results reveal the underlying physics of the confined electrons at MTBs of CDW metals, paving the way for the grain boundary engineering of the functionality.

Recent Progress in Two-Dimensional Material Exfoliation Technology and Enlightenment for Geological Sciences.

Mechanical exfoliation technology is vital for the development of two-dimensional (2D) materials. This technology has also facilitated the verification of the performance of electronic and optical devices made from 2D materials. In this Perspective, we provide an overview of exfoliation techniques and highlight key physical properties. Additionally, we explored the chemical instability of certain 2D materials and proposed practical solutions to enhance their stability. Furthermore, we discuss the advantages of suspended 2D materials, which demonstrate improved compatibility and properties compared to nonsuspended materials. A particularly intriguing aspect of this Perspective is the exploration of the similarities between the Earth's crust and 2D materials, offering insights into the formation mechanisms of geological phenomena. In this context, 2D materials may serve as simulators for studying geological processes. We hope that this Perspective stimulates further research into exfoliation technology and the physical/chemical properties of 2D materials while providing new inspiration for earth science investigations.

Robust Behavior of Charge Density Wave Quantum Motif Star-of-David in 2D NbSe2 Nanocrystals.

Charge density wave (CDW) is a typical collective phenomenon, and the phase change is generally accompanied by electronic transition with potential device applications. For the continuous miniaturization of devices, it is important to investigate the size effect down to the nanoscale. In this work, single-layer (SL) 1T-NbSe2 islands provide an ideal research platform to investigate the size effect on CDW arrangement and electronic states. The CDW motifs (Star-of-David [SOD]) at the island border are along the edge, and those at the interior tend to arrange in a triangular lattice for islands as small as 5 nm. Interestingly, in some small islands, the SOD clusters rearrange into a square-like lattice, and each SOD cluster remains robust as a quantum motif, both in the sense of geometry and electronic structures. Moreover, the electronic structure at the center of the small islands is downwards shifted compared to the big islands, explained by the spatial extension of the band bending originating from the edge of the islands. These findings reveal the robust behavior of CDW motifs down to the nanoscale and provide new insights into the size-limiting effect on 2D2D CDW ordering and electronic states down to a few nanometer extremes.

Observation of Two-Dimensional Type-II Superconductivity in Bulk 3R-TaSe2 by Scanning Tunneling Spectroscopy.

Here we report a low-temperature and vector-magnetic-field scanning tunneling microscopy/spectroscopy (STM/S) study on 3R-TaSe2. The sample surface was obtained by exfoliating a bulk 3R-TaSe2 single crystal in an ultrahigh-vacuum (UHV) chamber and then transferred in situ to STM. It was observed that the topmost layer shows a 3 × 3 charge density wave pattern at T = 4.2 K with metallic character in STS. The electronic characterization study by variable-temperature and magnetic field STS revealed that 3R-TaSe2 behaves as a type-II superconductor. More intriguingly, such superconductivity (SC) can survive under strong in-plane magnetic fields even up to 2.5 T and out-of-plane magnetic fields up to 0.7 T, exhibiting an anisotropic superconducting property. Temperature-dependent STS showed that 3R-TaSe2 undergoes a transition above 0.58 K. Our results may be important for understanding the intriguing SC properties of the 3R-phase van der Waals materials.

Strain Effects in Twisted Spiral Antimonene.

Van der Waals (vdW) layered materials exhibit fruitful novel physical properties. The energy band of such materials depends strongly on their structures, and a tremendous variation in their physical properties can be deduced from a tiny change in inter-layer spacing, twist angle, or in-plane strain. In this work, a kind of vdW layered material of spiral antimonene is constructed, and the strain effects in the material are studied. The spiral antimonene is grown on a germanium (Ge) substrate and is induced by a helical dislocation penetrating through few atomic-layers of antimonene (ß-phase). The as-grown spiral is intrinsically strained, and the lattice distortion is found to be pinned around the dislocation. Both spontaneous inter-layer twist and in-plane anisotropic strain are observed in scanning tunneling microscope (STM) measurements. The strain in the spiral antimonene can be significantly modified by STM tip interaction, leading to a variation in the surface electronic density of states (DOS) and a large modification in the work function of up to a few hundreds of millielectron-volts (meV). Those strain effects are expected to have potential applications in building up novel piezoelectric devices.

Multiple Electronic Phases Coexisting under Inhomogeneous Strains in the Correlated Insulator.

Monolayer transition metal dichalcogenides (TMDs) can host exotic phenomena such as correlated insulating and charge-density-wave (CDW) phases. Such properties are strongly dependent on the precise atomic arrangements. Strain, as an effective tuning parameter in atomic arrangements, has been widely used for tailoring material's structures and related properties, yet to date, a convincing demonstration of strain-induced dedicate phase transition at nanometer scale in monolayer TMDs has been lacking. Here, a strain engineering technique is developed to controllably introduce out-of-plane atomic deformations in monolayer CDW material 1T-NbSe2 . The scanning tunneling microscopy and spectroscopy (STM and STS) measurements, accompanied by first-principles calculations, demonstrate that the CDW phase of 1T-NbSe2 can survive under both tensile and compressive strains even up to 5%. Moreover, significant strain-induced phase transitions are observed, i.e., tensile (compressive) strains can drive 1T-NbSe2 from an intrinsic-correlated insulator into a band insulator (metal). Furthermore, experimental evidence of the multiple electronic phase coexistence at the nanoscale is provided. The results shed new lights on the strain engineering of correlated insulator and useful for design and development of strain-related nanodevices.

Orbital distortion and electric field control of sliding ferroelectricity in a boron nitride bilayer.

Recent experiments confirm that two-dimensional boron nitride (BN) films possess room-temperature out-of-plane ferroelectricity when each BN layer is sliding with respect to each other. This ferroelectricity is attributed to the interlayered orbital hybridization or interlayer charge transfer in previous work. In this work, we attempt to understand the sliding ferroelectricity from the perspective of orbital distortion of long-pair electrons. Using the maximally localized Wannier function method and first-principles calculations, the out-of-planepzorbitals of BN are investigated. Our results indicate that the interlayer van der Waals interaction causes the distortion of the Npzorbitals. Based on the picture of out-of-plane orbital distortion, we propose a possible mechanism to tune the ferroelectric polarization by external fields, including electric field and stress field. It is found that both the polarization intensity and direction can be modulated under the electric field. The polarization intensity of the system can also be controlled by stress field perpendicular to the plane. This study will provide theoretical help in the device design based on sliding ferroelectrics.

Optical bulk-boundary dichotomy in a quantum spin Hall insulator.

The bulk-boundary correspondence is a critical concept in topological quantum materials. For instance, a quantum spin Hall insulator features a bulk insulating gap with gapless helical boundary states protected by the underlying Z2 topology. However, the bulk-boundary dichotomy and distinction are rarely explored in optical experiments, which can provide unique information about topological charge carriers beyond transport and electronic spectroscopy techniques. Here, we utilize mid-infrared absorption micro-spectroscopy and pump-probe micro-spectroscopy to elucidate the bulk-boundary optical responses of Bi4Br4, a recently discovered room-temperature quantum spin Hall insulator. Benefiting from the low energy of infrared photons and the high spatial resolution, we unambiguously resolve a strong absorption from the boundary states while the bulk absorption is suppressed by its insulating gap. Moreover, the boundary absorption exhibits strong polarization anisotropy, consistent with the one-dimensional nature of the topological boundary states. Our infrared pump-probe microscopy further measures a substantially increased carrier lifetime for the boundary states, which reaches one nanosecond scale. The nanosecond lifetime is about one to two orders longer than that of most topological materials and can be attributed to the linear dispersion nature of the helical boundary states. Our findings demonstrate the optical bulk-boundary dichotomy in a topological material and provide a proof-of-principal methodology for studying topological optoelectronics.

Single-pixel imaging of a translational object.

Image-free tracking methods based on single-pixel detectors (SPDs) can track a moving object at a very high frame rate, but they rarely can achieve simultaneous imaging of such an object. In this study, we propose a method for simultaneously obtaining the relative displacements and images of a translational object. Four binary Fourier patterns and two differential Hadamard patterns are used to modulate one frame of the object and then modulated light signals are obtained by SPD. The relative displacements and image of the moving object can be gradually obtained along with the detection. The proposed method does not require any prior knowledge of the object and its motion. The method has been verified by simulations and experiments, achieving a frame rate of 3332 Hz to acquire relative displacements of a translational object at a spatial resolution of 128 × 128 pixels using a 20000-Hz digital micro-mirror device. This proposed method can broaden the application of image-free tracking methods and obtain spatial information about moving objects.

Ullmann-Like Covalent Bond Coupling without Participation of Metal Atoms.

Ullmann-like on-surface synthesis is one of the most appropriate approaches for the bottom-up fabrication of covalent organic nanostructures and many successes have been achieved. The Ullmann reaction requires the oxidative addition of a catalyst (a metal atom in most cases): the metal atom will insert into a carbon-halogen bond, forming organometallic intermediates, which are then reductively eliminated and form C-C covalent bonds. As a result, traditional Ullmann coupling involves reactions of multiple steps, making it difficult to control the final product. Moreover, forming the organometallic intermediates will potentially poison the metal surface catalytic reactivity. In the study, we used the 2D hBN, an atomically thin sp2-hybridized sheet with a large band gap, to protect the Rh(111) metal surface. It is an ideal 2D platform to decouple the molecular precursor from the Rh(111) surface while maintaining the reactivity of Rh(111). We realize an Ullmann-like coupling of a planar biphenylene-based molecule, i.e., 1,8-dibromobiphenylene (BPBr2), on an hBN/Rh(111) surface with an ultrahigh selectivity of the biphenylene dimer product, containing 4-, 6-, and 8-membered rings. The reaction mechanism, including electron wave penetration and the template effect of the hBN, is elucidated by combining low-temperature scanning tunneling microscopy and density functional theory calculations. Our findings are expected to play an essential role regarding the high-yield fabrication of functional nanostructures for future information devices.

Unveiling Electronic Behaviors in Heterochiral Charge-Density-Wave Twisted Stacking Materials with 1.25 nm Unit Dependence.

Layered charge-density-wave (CDW) materials have gained increasing interest due to their CDW stacking-dependent electronic properties for practical applications. Among the large family of CDW materials, those with star of David (SOD) patterns are very important due to the potentials for quantum spin liquid and related device applications. However, the spatial extension and the spin coupling information down to the nanoscale remain elusive. Here, we report the study of heterochiral CDW stackings in bilayer (BL) NbSe2 with high spatial resolution. We reveal that there exist well-defined heterochiral stackings, which have inhomogeneous electronic states among neighboring CDW units (star of David, SOD), significantly different from the homogeneous electronic states in the homochiral stackings. Intriguingly, the different electronic behaviors are spatially localized within each SOD with a unit size of 1.25 nm, and the gap sizes are determined by the different types of SOD stackings. Density functional theory (DFT) calculations match the experimental measurements well and reveal the SOD-stacking-dependent correlated electronic states and antiferromagnetic/ferromagnetic couplings. Our findings give a deep understanding of the spatial distribution of interlayer stacking and the delicate modulation of the spintronic states, which is very helpful for CDW-based nanoelectronic devices.

Composition and phase engineering of metal chalcogenides and phosphorous chalcogenides.

Two-dimensional (2D) materials with multiphase, multielement crystals such as transition metal chalcogenides (TMCs) (based on V, Cr, Mn, Fe, Cd, Pt and Pd) and transition metal phosphorous chalcogenides (TMPCs) offer a unique platform to explore novel physical phenomena. However, the synthesis of a single-phase/single-composition crystal of these 2D materials via chemical vapour deposition is still challenging. Here we unravel a competitive-chemical-reaction-based growth mechanism to manipulate the nucleation and growth rate. Based on the growth mechanism, 67 types of TMCs and TMPCs with a defined phase, controllable structure and tunable component can be realized. The ferromagnetism and superconductivity in FeXy can be tuned by the y value, such as superconductivity observed in FeX and ferromagnetism in FeS2 monolayers, demonstrating the high quality of as-grown 2D materials. This work paves the way for the multidisciplinary exploration of 2D TMPCs and TMCs with unique properties.