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The interplay between strong electron-electron interaction and symmetry breaking can have profound influence on the topological properties of materials. In magic angle twisted bilayer graphene (MATBG), the flat band with a single SU(4) flavor associated with the spin and valley degrees of freedom gains non-zero Chern number when C2z symmetry or C2zT symmetry is broken. Electron-electron interaction can further lift the SU(4) degeneracy, leading to the Chern insulator states. Here we report a complete sequence of zero-field Chern insulators at all odd integer fillings (v = +-1, +-3) with different chirality (C = 1 or -1) in hBN aligned MATBG which structurally breaks C2z symmetry. The Chern states at hole fillings (v = -1, -3), which are firstly observed in this work, host an opposite chirality compared with the electron filling scenario. By slightly doping the v = +-3 states, we have observed new correlated insulating states at incommensurate moir\'e fillings which is highly suggested to be intrinsic Wigner crystals according to our theoretical calculations. Remarkably, we have observed prominent Streda-formula violation around v = -3 state. By doping the Chern gap at v = -3 with notable number of electrons at finite magnetic field, the Hall resistance Ryx robustly quantizes to ~ h/e2 whereas longitudinal resistance Rxx vanishes, indicating that the chemical potential is pinned within a Chern gap, forming an incommensurate Chern insulator. By providing the first experimental observation of zero-field Chern insulators in the flat valence band, our work fills up the overall topological framework of MATBG with broken C2z symmetry. Our findings also demonstrate that doped topological flat band is an ideal platform to investigate exotic incommensurate correlated topological states., Comment: 28 pages. 5 figures

The extrinsic stacking sequence based on intrinsic crystal symmetry in multilayer two-dimensional materials plays a significant role in determining their electronic and optical properties. Compared with Bernal-stacked (ABA) multilayer graphene, rhombohedral (ABC) multilayer graphene hosts stronger electron-electron interaction due to its unique dispersion at low-energy excitations and has been utiliazed as a unique platform to explore strongly correlated physics. However, discerning the stacking sequence has always been a quite time-consuming process by scanning mapping methods. Here, we report a rapid recognition method for ABC- stacked graphene with high accuracy by infrared imaging based on the distinct optical responses at infrared range. The optical contrast of the image between ABC and ABA stacked graphene is strikingly clear, and the discernibility is comparable to traditional optical Raman microscopy but with higher consistency and throughput. We further demonstrate that the infrared imaging technique can be integrated with dry transfer techniques commonly used in the community. This rapid and convenient infrared imaging technique will significantly improve the sorting efficiency for differently stacked multilayer graphene, thereby accelerating the exploration of the novel emergent correlated phenomena in ABC stacked graphene.

Interlayer rotation in van der Waals (vdW) materials offers great potential for manipulating phonon dynamics and heat flow in advanced electronics with ever higher compactness and power density. However, despite extensive theoretical efforts in recent years, experimental measurements remain scarce especially due to the critical challenges of preparing single-crystalline twisted interfaces and probing interfacial thermal transport with sufficient resolution. Here, we exploited the intrinsic twisted interfaces in highly oriented pyrolytic graphite (HOPG). By developing novel experimental schemes based on microfabricated mesas, we managed to achieve simultaneous mechanical characterizations and thermal measurements. In particular, we pushed the HOPG mesas with a microprobe to identify and rotate single-crystalline intrinsic interfaces owing to their slippery nature as is well known in structural superlubricity. Remarkably, we observed over 30-fold suppression of thermal conductance for the slippery interfaces by using epitaxial graphite as a control. Nonetheless, the interfacial conductance remains around 600 $\mathrm{MWm^{-2}K^{-1}}$ which surpasses the highest values for artificially stacked vdW structures by more than five times. Further, atomic simulations revealed the predominant role of the transverse acoustic phonons. Together, our findings highlight a general physical picture that directly correlates interfacial thermal transport with sliding resistance, and lay the foundation for twist-enabled thermal management which are particularly beneficial to twistronics and slidetronics.

Fractional quantum anomalous hall effect (FQAHE), a transport effect with fractionally quantized Hall plateau emerging under zero magnetic field, provides a radically new opportunity to engineer topological quantum electronics. By construction of topological flat band with moire engineering, intrinsic FQAHE has been observed in twisted MoTe2 system and rhombohedral pentalayer graphene/hBN moire superlattices with anomalous Hall resistivity quantization number C <= 2/3 including the gapless composite Fermi-liquid state with C = 1/2. Here we experimentally demonstrate a new system of rhombohedral hexalayer graphene (RHG)/hBN moire superlattices showing both fractional and integer quantum anomalous Hall effects when the lowest flat Chern band is fractionally and fully filled at zero magnetic field. The zero-field Hall resistance Rho_xy = h/Ce2 is quantized to values corresponding to C = 3/5, 2/3, 5/7, 3/4, 7/9 and 1 at moire filling factors v = 3/5, 2/3, 5/7, 3/4, 7/9 and 1, respectively. Particularly, the C = 3/4 FQAHE state at v = 3/4 moire filling featuring a minimum of longitudinal resistance Rho_xx and fractionally quantized Hall resistance Rho_xy = 4h/3e2, is observed for the first time under zero magnetic field. Such a state may be similar to the C = 3/4 fractional quantum hall (FQHE) state recently observed at high magnetic fields9,10 and possibly host fractional charge excitations obeying non-Abelian statistics. By tuning the electrical and magnetic fields at 0 < v < 1, we have observed a sign reversal of the Hall resistivity for v = 2/3 state, indicating a transition from quasi-electron-like excitations to quasi-hole ones. Our experiment has established RHG/hBN moire superlattices a promising platform to explore quasi-particles with fractional charge excitations and non-Abelian anyons at zero magnetic field.

Electrons residing in flat-band system can play a vital role in triggering spectacular phenomenology due to relatively large interactions and spontaneous breaking of different degeneracies. In this work we demonstrate chirally twisted triple bilayer graphene, a new moir\'e structure formed by three pieces of helically stacked Bernal bilayer graphene, as a highly tunable flat-band system. In addition to the correlated insulators showing at integer moir\'e fillings, commonly attributed to interaction induced symmetry broken isospin flavors in graphene, we observe abundant insulating states at half-integer moir\'e fillings, suggesting a longer-range interaction and the formation of charge density wave insulators which spontaneously break the moir\'e translation symmetry. With weak out-of-plane magnetic field applied, as observed half-integer filling states are enhanced and more quarter-integer filling states appear, pointing towards further quadrupling moir\'e unit cells. The insulating states at fractional fillings combined with Hartree-Fock calculations demonstrate the observation of a new type of correlated charge density wave insulators in graphene and points to a new accessible twist manner engineering correlated moir\'e electronics.

Boron nitride (BN) is today considered as one of the most promising materials for many novel applications including bright single photon emission, deep UV opto-electronics, small sized solid-state neutron detector, and high-performance two-dimensional materials, etc. Despite the recent successful fabrication of large-area BN single-crystals (typically <= 5 atomic layers), the scalable growth of thicker single-crystalline BN films still constitutes a great challenge. In this work, we demonstrate an approach to grow large-area multilayer single-crystal BN films by chemical vapor deposition on face-centered cubic Fe-Ni (111) single crystal alloy thin films with different stoichiometric phases. We show that the BN growth is greatly tunable and improved by increasing the Fe content in single-crystal Fe-Ni (111). The formation of pyramid-shaped multilayer BN domains with aligned orientation enables a continuous connection following a layer-by-layer, 'first-meet-first-connect', mosaic stitching mechanism. By means of selected area electron diffraction, micro-photoluminescence spectroscopy in the deep UV and high-resolution transmission electron microscopy, the layer-by-layer connection mechanism is unambiguously evidenced, and the stacking order has been verified to occur as unidirectional AB and ABC stackings, i.e., in the Bernal and rhombohedral BN phase.

Interfacial ferroelectricity emerges in heterostructures consisting of nonpolar van der Waals (vdW) layers, greatly expanding the scope of two dimensional ferroelectrics. In particular, the unconventional moire ferroelectricity observed in bilayer graphene/boron nitride (BN) heterostructures, exhibits promising functionalities with topological current, superconductivity and synaptic responses. However, the debate about its mechanism - correlation driven charge transfer between two graphene layers - limits device reproducibility and hence large-scale production. Here by designing a single-layer graphene encapsulated by lattice-mismatched WSe2, we identify the ferroelectricity as stemming from - instead of graphene moire bands - the particular BN, where interfacial sliding ferroelectricity must play a role. With similar structures, multilayer twisted MoS2 is found to reproduce the ferroelectricity. The key is a conductive moire ferroelectric, where the screened gate and the pinned domain wall together result in unchanged electronic states, i.e. anomalous screening. The intimate connection to interfacial sliding ferroelectricity thus provides advantages of diverse choices of constituent materials and robust polarization switching while preserving the unique anomalous screening, paving the way to reproducible and reliable memory-based devices in artificial intelligence.

Ferroelectric materials with switchable electric polarization hold great promise for a plethora of emergent applications, such as post-Moore's law nanoelectronics, beyond-Boltzmann transistors, non-volatile memories, and above-bandgap photovoltaic devices. Recent advances have uncovered an exotic sliding ferroelectric mechanism, which endows to design atomically thin ferroelectrics from non-ferroelectric parent monolayers. Although notable progress has been witnessed in understanding its fundamental properties, functional devices based on sliding ferroelectrics, the key touchstone toward applications, remain elusive. Here, we demonstrate the rewritable, non-volatile memory devices at room-temperature utilizing a two-dimensional (2D) sliding ferroelectric semiconductor of rhombohedral-stacked bilayer molybdenum disulfide. The 2D sliding ferroelectric memories (SFeMs) show superior performances with a large memory window of >8V, a high conductance ratio of above 106, a long retention time of >10 years, and a programming endurance greater than 104 cycles. Remarkably, flexible SFeMs are achieved with state-of-the-art performances competitive to their rigid counterparts and maintain their performances post bending over 103 cycles. Furthermore, synapse-specific Hebbian forms of plasticity and image recognition with a high accuracy of 97.81% are demonstrated based on flexible SFeMs. Our work demonstrates the sliding ferroelectric memories and synaptic plasticity on both rigid and flexible substrates, highlighting the great potential of sliding ferroelectrics for emerging technological applications in brain-inspired in-memory computing, edge intelligence and energy-efficient wearable electronics., Comment: 16 pages, 4 figures

The nonvolatile magnetoresistive random access memory (MRAM) is believed to facilitate emerging applications, such as in memory computing, neuromorphic computing and stochastic computing. Two dimensional (2D) materials and their van der Waals heterostructures promote the development of MRAM technology, due to their atomically smooth interfaces and tunable physical properties. Here we report the all-2D magnetoresistive memories featuring all electrical data reading and writing at room temperature based on WTe2/Fe3GaTe2/BN/Fe3GaTe2 heterostructures. The data reading process relies on the tunnel magnetoresistance of Fe3GaTe2/BN/Fe3GaTe2. The data writing is achieved through current induced polarization of orbital magnetic moments in WTe2, which exert torques on Fe3GaTe2, known as the orbit transfer torque (OTT) effect. In contrast to the conventional reliance on spin moments in spin transfer torque and spin orbit torque, the OTT effect leverages the natural out of plane orbital moments, facilitating field-free perpendicular magnetization switching through interface currents. Our results indicate that the emerging OTT MRAM is promising for low power, high performance memory applications.

Two-dimensional (2D) materials have received extensive research attentions over the past two decades due to their intriguing physical properties (such as the ultrahigh mobility and strong light-matter interaction at atomic thickness) and a broad range of potential applications (especially in the fields of electronics and optoelectronics). The growth of single-crystal 2D materials is the prerequisite to realize 2D-based high-performance applications. In this review, we aim to provide an in-depth analysis of the state-of-the-art technology for the growth and applications of 2D materials, with particular emphasis on single crystals. We first summarize the major growth strategies for monolayer 2D single crystals. Following that, we discuss the growth of multilayer single crystals, including the control of thickness, stacking sequence, and heterostructure composition. Then we highlight the exploration of 2D single crystals in electronic and optoelectronic devices. Finally, a perspective is given to outline the research opportunities and the remaining challenges in this field.

Optical nonlinearities, one of the most fascinating properties of two-dimensional (2D) materials, are essential for exploring novel physics in 2D systems and developing next-generation nonlinear optical applications. While tremendous efforts have been made to discover and optimize second-order nonlinear optical responses in various 2D materials, higher odd-order nonlinear processes, which are in general much less efficient than second order ones, have been paid less attention despite their scientific and applicational significance. Here we report giant odd-order nonlinear optical wave mixing in a correlated van der Waals insulator MnPSe3 at room temperature. Illuminated by two near-infrared femtosecond lasers simultaneously, it generates a series of degenerate and non-degenerate four- and six-wave mixing outputs, with conversion efficiencies up to the order of $10^{-4}$ and $10^{-6}$ for the four- and six-wave mixing processes, respectively, far exceeding the efficiencies of several prototypical nonlinear optical materials (GaSe, LiNbO3). This work highlights the intriguing prospect of transition metal phosphorous trichalcogenides for future research of the nonlinear light matter interactions in 2D systems and for potential nonlinear photonic applications., Comment: 17 pages, 4 figures

Optical neural networks (ONNs) herald a new era in information and communication technologies and have implemented various intelligent applications. In an ONN, the activation function (AF) is a crucial component determining the network performances and on-chip AF devices are still in development. Here, we first demonstrate on-chip reconfigurable AF devices with phase activation fulfilled by dual-functional graphene/silicon (Gra/Si) heterojunctions. With optical modulation and detection in one device, time delays are shorter, energy consumption is lower, reconfigurability is higher and the device footprint is smaller than other on-chip AF strategies. The experimental modulation voltage (power) of our Gra/Si heterojunction achieves as low as 1 V (0.5 mW), superior to many pure silicon counterparts. In the photodetection aspect, a high responsivity of over 200 mA/W is realized. Special nonlinear functions generated are fed into a complex-valued ONN to challenge handwritten letters and image recognition tasks, showing improved accuracy and potential of high-efficient, all-component-integration on-chip ONN. Our results offer new insights for on-chip ONN devices and pave the way to high-performance integrated optoelectronic computing circuits.

Optical phase-matching involves establishing a proper phase relationship between the fundamental and generated waves to enable efficient optical parametric processes. It is typically achieved through either birefringence or periodically assigned polarization. Here, we report that twist angle in two-dimensional (2D) materials can generate a nonlinear Berry optical phase to compensate the phase mismatch in the process of nonlinear optical frequency conversion, and the vertical assembly of 2D layers with a proper twist sequence will generate a nontrivial "twist-phase-matching" (twist-PM) regime. The twist-PM model offers superior flexibility in the design of optical crystals, which works for twisted layers with either periodic or random thickness distribution. The designed crystals from twisted rhombohedra boron nitride films give rise to a second-harmonic generation conversion efficiency of ~8% within a thickness of only 3.2 um, and a facile polarization controllability that is absent in conventional crystals (from linear to left-/right-handed circular/elliptical polarizations). Our methodology establishes a platform for the rational designing and atomic manufacturing of nonlinear optical crystals based on abundant 2D materials for various functionalities.

Berry curvature dipole plays an important role in various nonlinear quantum phenomena. However, the maximum symmetry allowed for nonzero Berry curvature dipole in the transport plane is a single mirror line, which strongly limits its effects in materials. Here, via probing the nonlinear Hall effect, we demonstrate the generation of Berry curvature dipole by applied dc electric field in WTe2, which is used to break the symmetry constraint. A linear dependence between the dipole moment of Berry curvature and the dc electric field is observed. The polarization direction of the Berry curvature is controlled by the relative orientation of the electric field and crystal axis, which can be further reversed by changing the polarity of the dc field. Our Letter provides a route to generate and control Berry curvature dipole in broad material systems and to facilitate the development of nonlinear quantum devices.

Natural materials usually consist of isotopic mixtures, for which different isotopic ratios can lead to distinct material properties such as thermal conductivity and nucleation process. However, the knowledge of isotopic interface remains largely unexplored mainly due to the challenges in isotopic identification and property measurement at an atomic scale. Here, by using monochromated electron energy-loss spectroscopy in a scanning transmission electron microscope, we reveal momentum-transfer-dependent lattice vibration behavior at an artificial h-10BN/h-11BN heterostructure with sub-unit-cell resolution. We find the vibrational energy changes across the isotopic interface gradually, featuring a wide transition regime, which suggests strong delocalization of the out-of-plane optical phonons at the interface. In addition, we identify phonons near the Brillouin zone center have a transition regime ~3.34 nm (10 atomic layers), whereas phonons at the Brillouin zone boundary transition in ~1.66 nm (5 atomic layers). We propose that the isotope-induced charge effect at the interface accounts for the distinct delocalization behavior. Moreover, intra-atomic layer variation of vibration energy is also sensitive to the momentum transfer, thus at the interface it depends on both of momentum transfer and mass change. The revealed lattice vibration behavior at an isotopic interface provides new insights to understand the isotopic effects on properties in natural materials.

In twisted h-BN/graphene heterostructures, the complex electronic properties of the fast-traveling electron gas in graphene are usually considered to be fully revealed. However, the randomly twisted heterostructures may also have unexpected transition behaviors, which may influence the device performance. Here, we study the twist angle-dependent coupling effects of h-BN/graphene heterostructures using monochromatic electron energy loss spectroscopy. We find that the moir\'e potentials alter the band structure of graphene, resulting in a redshift of the intralayer transition at the M-point, which becomes more pronounced up to 0.25 eV with increasing twist angle. Furthermore, the twisting of the Brillouin zone of h-BN relative to the graphene M-point leads to tunable vertical transition energies in the range of 5.1-5.6 eV. Our findings indicate that twist-coupling effects of van der Waals heterostructures should be carefully considered in device fabrications, and the continuously tunable interband transitions through the twist angle can serve as a new degree of freedom to design optoelectrical devices.

Missing second-order nonlinearity in centrosymmetric graphene overshadows its intriguing optical attribute. Here, we report redox-governed charge doping could effectively break the centrosymmetry of bilayer graphene (BLG), enabling a strong second harmonic generation (SHG) with a strength close to that of the well-known monolayer MoS2. Verified from control experiments with in situ electrical current annealing and electrically gate-controlled SHG, the required centrosymmetry breaking of the emerging SHG arises from the charge-doping on the bottom layer of BLG by the oxygen/water redox couple. Our results not only reveal that charge doping is an effective way to break the inversion symmetry of BLG despite its strong interlayer coupling but also indicate that SHG spectroscopy is a valid technique to probe molecular doping on two-dimensional materials.

Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline substrates. However, in principle, this success in monolayer epitaxy seems extremely difficult to be replicated to bi- or few-layer growth, as the full coverage of the first layer was believed to terminate the reactivity of those adopting catalytic metal surfaces. Here, we report an exceptional layer-by-layer chemical vapour deposition (CVD) growth of large size bi-layer graphene single-crystals, enabled by self-transmitting catalytic activity from platinum (Pt) surfaces to the outermost graphene layers. In-situ growth and real-time surveillance experiments, under well-controlled environments, unambiguously verify that the growth does follow the layer-by-layer mode on open surfaces of MLG/Pt(111). First-principles calculations indicate that the transmittal of catalytic activity is allowed by an appreciable electronic hybridisation between graphene overlayers and Pt surfaces, enabling catalytic dissociation of hydrocarbons and subsequently direct graphitisation of their radicals on the outermost sp2 carbon surface. This self-transmitting catalytic activity is also proven to be robust for tube-furnace CVD in fabricating single-crystalline graphene bi-, tri- and tetra-layers, as well as h-BN few-layers. Our findings offer an exceptional strategy for potential controllable, layer-by-layer and wafer-scale growth of vertically stacked few-layered 2D single crystals., Comment: 5 figures and 9 extended figures

Two-dimensional (2D) semiconductor of MoS2 has great potential for advanced electronics technologies beyond silicon1-9. So far, high-quality monolayer MoS2 wafers10-12 are already available and various demonstrations from individual transistors to integrated circuits have also been shown13-15. In addition to the monolayer, multilayers have narrower band gaps but improved carrier mobilities and current capacities over the monolayer5,16-18. However, achieving high-quality multilayer MoS2 wafers remains a challenge. Here we report the growth of high quality multilayer MoS2 4-inch wafers via the layer-by-layer epitaxy process. The epitaxy leads to well-defined stacking orders between adjacent epitaxial layers and offers a delicate control of layer numbers up to 6. Systematic evaluations on the atomic structures and electronic properties were carried out for achieved wafers with different layer numbers. Significant improvements on device performances were found in thicker-layer field effect transistors (FETs), as expected. For example, the average field-effect mobility ({\mu}FE) at room temperature (RT) can increase from ~80 cm2V-1s-1 for monolayer to ~110/145 cm2V-1s-1 for bilayer/trilayer devices. The highest RT {\mu}FE=234.7 cm2V-1s-1 and a record-high on-current densities of 1.704 mA{\mu}m-1 at Vds=2 V were also achieved in trilayer MoS2 FETs with a high on/off ratio exceeding 107. Our work hence moves a step closer to practical applications of 2D MoS2 in electronics., Comment: 13 pages,4 Figures

The reversal of perpendicular magnetization (PM) by electric control is crucial for high-density integration of low-power magnetic random-access memory (MRAM). Although the spin-transfer torque (STT) and spin-orbit torque (SOT) technologies have been used to switch the magnetization of a free layer with perpendicular magnetic anisotropy, the former has limited endurance because of the high current density directly through the junction, while the latter requires an external magnetic field or unconventional configuration to break the symmetry. Here we propose and realize the orbit-transfer torque (OTT), that is, exerting torque on the magnetization using the orbital magnetic moments, and thus demonstrate a new strategy for current-driven PM reversal without external magnetic field. The perpendicular polarization of orbital magnetic moments is generated by a direct current in a few-layer WTe2 due to the existence of nonzero Berry curvature dipole, and the polarization direction can be switched by changing the current polarity. Guided by this principle, we construct the WTe2/Fe3GeTe2 heterostructures, where the OTT driven field-free deterministic switching of PM is achieved.

Hyperbolic metasurfaces based on van der Waals (vdW) materials support propagation of extremely anisotropic polaritons towards nanoscale light compression and manipulation, and thus has great potential in the applications of planar hyperlens, nanolasing, quantum optics and ultrasensitive infrared spectroscopy. Two-dimensional hexagonal boron nitride (h-BN) as a vdW metasurface can manipulate the propagation of hyperbolic polaritons at the level of single atomic layers, possessing higher degree of field confinement and lower losses than the conventional media. However, active manipulation of hyperbolic polaritonic waves in h-BN midinfrared metasurfaces remains elusive. Herein, we provide an effective strategy for constructing tunable mid-infrared hyperbolic vdW metasurfaces (HMSs). They are composed of meta-atoms that are the in-plane heterostructures of thin-layer h-BN and monolayer graphene strips (iHBNG). The strong coupling of h-BN phonons and graphene plasmons enables the large tunability of light fields by tailoring chemical potentials of graphene without frequency shift, which involves topological transitions of polaritonic modes, unidirectional polariton propagation and local-density-of-state enhancement. Simulated visual near-field distributions of iHBNG metasurfaces reveal the unique transformations of hyperbolic polariton propagations, distinguished from that of individual h-BN and graphene metasurfaces. Our findings provide a platform of optical nanomanipulation towards emerging on-chip polaritonic devices., Comment: 23 pages, 4 figures

We report the strong dependence of resistance on uniaxial strain in monolayer WSe2 at various temperatures, where the gauge factor can reach as large as 2400. The observation of strain-dependent resistance and giant gauge factor is attributed to the emergence of nonzero Berry curvature dipole. Upon increasing strain, Berry curvature dipole can generate net orbital magnetization, which would introduce additional magnetic scattering, decreasing the mobility and thus conductivity. Our work demonstrates the strain engineering of Berry curvature and thus the transport properties, making monolayer WSe2 potential for the application in the high-performance flexible and transparent electronics., Comment: 15 pages, 4 figures

The breakdown of translational symmetry at heterointerfaces leads to the emergence of new phonon modes localized near the interface. These interface phonons play an essential role in thermal/electrical transport properties in devices especially in miniature ones wherein the interface may dominate the entire response of the device. Knowledge of phonon dispersion at interfaces is therefore highly desirable for device design and optimization. Although theoretical work has begun decades ago, experimental research is totally absent due to challenges in achieving combined spatial, momentum and spectral resolutions required to probe localized phonon modes. Here we use electron energy loss spectroscopy in an electron microscope to directly measure both the local phonon density of states and the interface phonon dispersion relation for an epitaxial cBN-diamond heterointerface. In addition to bulk phonon modes, we observe acoustic and optical phonon modes localized at the interface, and modes isolated away from the interface. These features only appear within ~ 1 nm around the interface. The experimental results can be nicely reproduced by ab initio calculations. Our findings provide insights into lattice dynamics at heterointerfaces and should be practically useful in thermal/electrical engineering.

Flexoelectricity is a type of ubiquitous and prominent electromechanical coupling, pertaining to the response of electrical polarization to mechanical strain gradients while not restricted to the symmetry of materials. However, large elastic deformation in most solids is usually difficult to achieve and the strain gradient at minuscule is challenging to control. Here we exploit the exotic structural inhomogeneity of grain boundary to achieve a huge strain gradient (~ 1.2 nm-1) within 3 ~ 4 unit-cells, and thus obtain atomic-scale flexoelectric polarization up to ~ 38 {\mu}C/cm2 at a 24 LaAlO3 grain boundary. The nanoscale flexoelectricity also modifies the electrical activity of grain boundaries. Moreover, we prove that it is a general and feasible way to form large strain gradients at atomic scale by altering the misorientation angles of grain boundaries in different dielectric materials. Thus, engineering of grain boundaries provides an effective pathway to achieve tunable flexoelectricity and broadens the electromechanical functionalities of non-piezoelectric materials., Comment: 16 pages,4 figures

Room-temperature polar skyrmion bubbles that are recently found in oxide superlattice, have received enormous interests for their potential applications in nanoelectronics due to the nanometer size, emergent chirality, and negative capacitance. For practical applications, the ability to controllably manipulate them by using external stimuli is prerequisite. Here, we study the dynamics of individual polar skyrmion bubbles at the nanoscale by using in situ biasing in a scanning transmission electron microscope. The reversible electric field-driven phase transition between topological and trivial polar states are demonstrated. We create, erase and monitor the shrinkage and expansion of individual polar skyrmions. We find that their transition behaviors are substantially different from that of magnetic analogue. The underlying mechanism is discussed by combing with the phase-field simulations. The controllable manipulation of nanoscale polar skyrmions allows us to tune the dielectric permittivity at atomic scale and detailed knowledge of their phase transition behaviors provides fundamentals for their applications in nanoelectronics.

Understanding the atomic structure and structural instability of organic-inorganic hybrid perovskites is the key to appreciate their remarkable photoelectric properties and failure mechanism. Here, using low-dose imaging technique by direct-detection electron-counting camera in transmission electron microscope, we investigate the atomic structure and decomposition pathway of CH3NH3PbI3 (MAPbI3) at the atomic scale. We successfully image the atomic structure of perovskite in real space under ultra-low electron dose condition, and observe a two-step decomposition process, i.e. initial loss of MA followed by the collapse of perovskite structure into 6H-PbI2 with their critical threshold dose also determined. Interestingly, an intermediate phase (MA0.5PbI3) with locally ordered vacancies can robustly exist before perovskite collapses, enlightening strategies for prevention and recovery of perovskite structure during degradation. Associated with structure evolution, the bandgap gradually increases from ~1.6 eV to ~2.1 eV, and it is found that both C-N and N-H bonds can be destroyed under irradiation, releasing NH3 and leaving hydrocarbons. These findings enhance our understanding of the photoelectric properties and failure mechanism of MAPbI3, providing potential strategy into material optimization.

Topological polar vortices that are the electric analogues of magnetic objects, present great potential in applications of future nanoelectronics due to their nanometer size, anomalous dielectric response, and chirality. To enable the functionalities, it is prerequisite to manipulate the polar states and chirality by using external stimuli. Here, we probe the evolutions of polar state and chirality of polar vortices in PbTiO3/SrTiO3 superlattices under electric field by using atomically resolved in situ scanning transmission electron microscopy and phase-field simulations. We find that the adjacent clockwise and counterclockwise vortex usually have opposite chirality. The phase-field simulations suggest that the rotation reversal or axial polarization switching can lead to the chirality change. Guided by which, we experimentally validate that the vortex rotation direction can be changed by applying and subsequently removing of electric fields, offering a potential strategy to manipulate the vortex chirality. The revealed details of dynamic behavior for individual polar vortices at atomic scale and the proposed strategy for chirality manipulation provide fundamentals for future device applications.

The electronic topology is generally related to the Berry curvature, which can induce the anomalous Hall effect in time-reversal symmetry breaking systems. Intrinsic monolayer transition metal dichalcogenides possesses two nonequivalent K and K' valleys, having Berry curvatures with opposite signs, and thus vanishing anomalous Hall effect in this system. Here we report the experimental realization of asymmetrical distribution of Berry curvature in a single valley in monolayer WSe2 through applying uniaxial strain to break C3v symmetry. As a result, although the Berry curvature itself is still opposite in K and K' valleys, the two valleys would contribute equally to nonzero Berry curvature dipole. Upon applying electric field, the emergent Berry curvature dipole would lead to an out-of-plane orbital magnetization, which further induces an anomalous Hall effect with a linear response to E^2, known as nonlinear Hall effect. We show the strain modulated transport properties of nonlinear Hall effect in monolayer WSe2 with moderate hole-doping by gating. The second-harmonic Hall signals show quadratic dependence on electric field, and the corresponding orbital magnetization per current density can reach as large as 60. In contrast to the conventional Rashba-Edelstein effect with in-plane spin polarization, such current-induced orbital magnetization is along the out-of-plane direction, thus promising for high-efficient electrical switching of perpendicular magnetization.

There is a rising prospective in harvesting energy from water droplets, as microscale energy is required for the distributed sensors in the interconnected human society. However, achieving a sustainable direct-current generating device from water flow is rarely reported, and the quantum polarization principle of the water molecular remains uncovered. Herein, we propose a dynamic water-semiconductor junction with moving water sandwiched between two semiconductors as a moving dielectric medium, which outputs a sustainable direct-current voltage of 0.3 V and current of 0.64 uA with low internal resistance of 390 kilohm. The sustainable direct-current electricity is originating from the dynamic water polarization process in water-semiconductor junction, in which water molecules are continuously polarized and depolarized driven by the mechanical force and Fermi level difference, during the movement of the water on silicon. We further demonstrated an encapsulated portable power-generating device with simple structure and continuous direct-current voltage, which exhibits its promising potential application in the field of wearable electronic generators.

Nontrivial topological structures offer rich playground in condensed matter physics including fluid dynamics, superconductivity, and ferromagnetism, and they promise alternative device configurations for post-Moore spintronics and electronics. Indeed, magnetic skyrmions are actively pursued for high-density data storage, while polar vortices with exotic negative capacitance may enable ultralow power consumption in microelectronics. Following extensive investigations on a variety of magnetic textures including vortices, domain walls and skyrmions in the past decades, studies on polar topologies have taken off in recent years, resulting in discoveries of closure domains, vortices, and skyrmions in ferroelectric materials. Nevertheless, the atomic-scale creation of topological polar structures is largely confined in a single ferroelectric system, PbTiO3 (PTO) with large polarization, casting doubt on the generality of polar topologies and limiting their potential applications. In this work, we successfully create previously unrealized atomic-scale polar antivortices in the nominally nonpolar SrTiO3 (STO), expanding the reaches of topological structures and completing an important missing link in polar topologies. The work shed considerable new insight into the formation of topological polar structures, and offers guidance in searching for new polar textures.

The capture of photoexcited deep-band hot carriers, excited by photons with energies far above the bandgap, is of significant importance for photovoltaic and photoelectronic applications since it is directly related to the quantum efficiency of photon-to-electron conversion. By employing time-resolved photoluminescence and state-of-the-art time-domain density functional theory, we reveal that photoexcited hot carriers in organic-inorganic hybrid perovskites prefer a zigzag interfacial charge-transfer pathway, i.e., the hot carriers transfer back and forth between CH3NH3PbI3 and graphene, before they reach a charge separated state. Driven by quantum coherence and interlayer vibrational modes, this pathway at the semiconductor-graphene interface takes about 400 femtoseconds, much faster than the relaxation process within CH3NH3PbI3 (in several picoseconds). We further demonstrate that the transfer rate of the pathway can be further enhanced by interfacial defects. Our work provides a new insight for the fundamental understanding and precise manipulation of hot-carrier dynamics at the complex semiconductor-graphene interfaces, paving the way for highly efficient photovoltaic and photoelectric device optimization.

Liquid electricity generator and hydrovoltaic technology have received numerous attentions, which can be divided into horizontal movement generator and vertical movement generator. The horizontal movement generator is limited for powering the integrated and miniaturized energy chip as the current output direction is depending on the moving direction of the water droplet, which means a sustainable and continuous direct-current (DC) electricity output can be hardly achieved because of the film of limited length. On the other hand, the existing vertical movement generators include triboelectricity or humidity gradient-based liquid electricity generator, where the liquid or water resource must be sustainably supplied to ensure continuous current output. Herein, we have designed an integratable vertical generator by sandwiching water droplets with semiconductor and metal, such as graphene or aluminum. This generator, named as polarized liquid molecular generator (PLMG), directly converts the lateral kinetic energy of water droplet into vertical DC electricity with an output voltage of up to ~1.0 V from the dynamic water-semiconductor interface. The fundamental discovery of PLMG is related to the non-symmetric structure of liquid molecules, such as water and alcohols, which can be polarized under the guidance of built-in field caused by the Fermi level difference between metal and semiconductor, while the symmetric liquid molecules cannot produce any electricity on the opposite. Integratable PLMG with a large output power of ~90 nW and voltage of ~2.7 V has been demonstrated, meanwhile its small internal resistance of ~250 kilohm takes a huge advantage in resistance matching with the impedance of electron components. The PLMG shows potential application value in the Internet of Things (IoTs) after proper miniaturization and integration.

Here, in an effort towards facile and fast screening/diagnosis of novel coronavirus disease 2019 (COVID-19), we combined the unprecedently sensitive graphene field-effect transistor (Gr-FET) with highly selective antibody-antigen interaction to develop a coronavirus immunosensor. The Gr-FET immunosensors can rapidly identify (about 2 mins) and accurately capture the COVID-19 spike protein S1 (which contains a receptor binding domain, RBD) at a limit of detection down to 0.2 pM, in a real-time and label-free manner. Further results ensure that the Gr-FET immunosensors can be promisingly applied to screen for high-affinity antibodies (with binding constant up to 2*10^11 M^-1 against the RBD) at concentrations down to 0.1 pM. Thus, our developed electrical Gr-FET immunosensors provide an appealing alternative to address the early screening/diagnosis as well as the analysis and rational design of neutralizing-antibody locking methods of this ongoing public health crisis., Comment: 2 figures

Contact interface properties are important in determining the performances of devices based on atomically thin two-dimensional (2D) materials, especially those with short channels. Understanding the contact interface is therefore quite important to design better devices. Herein, we use scanning transmission electron microscopy, electron energy loss spectroscopy, and first-principles calculations to reveal the electronic structures within the metallic (1T')-semiconducting (2H) MoTe2 coplanar phase boundary across a wide spectral range and correlate its properties and atomic structure. We find that the 2H-MoTe2 excitonic peaks cross the phase boundary into the 1T' phase within a range of approximately 150 nm. The 1T'-MoTe2 crystal field can penetrate the boundary and extend into the 2H phase by approximately two unit cells. The plasmonic oscillations exhibit strong angle dependence, i.e., a red-shift (approximately 0.3 eV-1.2 eV) occurs within 4 nm at 1T'/2H-MoTe2 boundaries with large tilt angles, but there is no shift at zero-tilted boundaries. These atomic-scale measurements reveal the structure-property relationships of 1T'/2H-MoTe2 boundary, providing useful information for phase boundary engineering and device development based on 2D materials., Comment: 14 pages and 4 figures. National Science Review 2020

The ability to controllably manipulate the complex topological polar configurations, such as polar flux-closure via external stimuli, enables many applications in electromechanical devices and nanoelectronics including high-density information storage. Here, by using the atomically resolved in situ scanning transmission electron microscopy, we find that a polar flux-closure structure in PbTiO3/SrTiO3 superlattices films can be reversibly switched to ordinary mono ferroelectric c domain or a domain under electric field or stress. Specifically, the electric field initially drives the flux-closure move and breaks them to form intermediate a/c striped domains, while the mechanical stress firstly starts to squeeze the flux-closures to convert into small vortices at the interface and form a continues dipole wave. After the removal of the external stimuli, the flux-closure structure spontaneously returns. Our atomic study provides valuable insights into understanding the lattice-charge interactions and the competing interactions balance in these complex topological structures. Such reversible switching between the flux-closure and ordinary ferroelectric domains also provides the foundation for applications such as memories and sensors., Comment: 22 pages, 5figures