On-device phase engineering.

In situ tailoring of two-dimensional materials' phases under external stimulus facilitates the manipulation of their properties for electronic, quantum and energy applications. However, current methods are mainly limited to the transitions among phases with unchanged chemical stoichiometry. Here we propose on-device phase engineering that allows us to realize various lattice phases with distinct chemical stoichiometries. Using palladium and selenide as a model system, we show that a PdSe2 channel with prepatterned Pd electrodes can be transformed into Pd17Se15 and Pd4Se by thermally tailoring the chemical composition ratio of the channel. Different phase configurations can be obtained by precisely controlling the thickness and spacing of the electrodes. The device can be thus engineered to implement versatile functions in situ, such as exhibiting superconducting behaviour and achieving ultralow-contact resistance, as well as customizing the synthesis of electrocatalysts. The proposed on-device phase engineering approach exhibits a universal mechanism and can be expanded to 29 element combinations between a metal and chalcogen. Our work highlights on-device phase engineering as a promising research approach through which to exploit fundamental properties as well as their applications.

Interfacial magnetic spin Hall effect in van der Waals Fe3GeTe2/MoTe2 heterostructure.

The spin Hall effect (SHE) allows efficient generation of spin polarization or spin current through charge current and plays a crucial role in the development of spintronics. While SHE typically occurs in non-magnetic materials and is time-reversal even, exploring time-reversal-odd (T-odd) SHE, which couples SHE to magnetization in ferromagnetic materials, offers a new charge-spin conversion mechanism with new functionalities. Here, we report the observation of giant T-odd SHE in Fe3GeTe2/MoTe2 van der Waals heterostructure, representing a previously unidentified interfacial magnetic spin Hall effect (interfacial-MSHE). Through rigorous symmetry analysis and theoretical calculations, we attribute the interfacial-MSHE to a symmetry-breaking induced spin current dipole at the vdW interface. Furthermore, we show that this linear effect can be used for implementing multiply-accumulate operations and binary convolutional neural networks with cascaded multi-terminal devices. Our findings uncover an interfacial T-odd charge-spin conversion mechanism with promising potential for energy-efficient in-memory computing.

Highly Stable HfO2 Memristors through van der Waals Electrode Lamination and Delamination.

Memristors have attracted considerable attention in the past decade, holding great promise for future neuromorphic computing. However, the intrinsic poor stability and large device variability remain key limitations for practical application. Here, we report a simple method to directly visualize the origin of poor stability. By mechanically removing the top electrodes of memristors operated at different states (such as SET or RESET), the memristive layer could be exposed and directly characterized through conductive atomic force microscopy, providing two-dimensional area information within memristors. Based on this technique, we observed the existence of multiple conducting filaments during the formation process and built up a physical model between filament numbers and the cycle-to-cycle variation. Furthermore, by improving the interface quality through the van der Waals top electrode, we could reduce the filament number down to a single filament during all switching cycles, leading to much controlled switching behavior and reliable device operation.

Parallel perception of visual motion using light-tunable memory matrix.

Parallel perception of visual motion is of crucial significance to the development of an intelligent machine vision system. However, implementing in-sensor parallel visual motion perception using conventional complementary metal-oxide semiconductor technology is challenging, because the temporal and spatial information embedded in motion cannot be simultaneously encoded and perceived at the sensory level. Here, we demonstrate the parallel perception of diverse motion modes at the sensor level by exploiting light-tunable memory matrix in a van der Waals (vdW) heterostructure array. The optoelectronic characteristics of gate-tunable photoconductivity and light-tunable memory matrix enable devices in the array to realize simultaneous encoding and processing of incoming spatiotemporal light pattern. Furthermore, we implement a visual motion perceptron with the array capable of deciphering multiple motion parameters in parallel, including direction, velocity, acceleration, and angular velocity. Our work opens up a promising venue for the realization of an intelligent machine vision system based on in-sensor motion perception.

Cascadable in-memory computing based on symmetric writing and readout.

The building block of in-memory computing with spintronic devices is mainly based on the magnetic tunnel junction with perpendicular interfacial anisotropy (p-MTJ). The resulting asymmetric write and readout operations impose challenges in downscaling and direct cascadability of p-MTJ devices. Here, we propose that a previously unimplemented symmetric write and readout mechanism can be realized in perpendicular-anisotropy spin-orbit (PASO) quantum materials based on Fe3GeTe2 and WTe2. We demonstrate that field-free and deterministic reversal of the perpendicular magnetization can be achieved using unconventional charge-to-z-spin conversion. The resulting magnetic state can be readily probed with its intrinsic inverse process, i.e., z-spin-to-charge conversion. Using the PASO quantum material as a fundamental building block, we implement the functionally complete set of logic-in-memory operations and a more complex nonvolatile half-adder logic function. Our work highlights the potential of PASO quantum materials for the development of scalable energy-efficient and ultrafast spintronic computing.

Tunable quantum criticalities in an isospin extended Hubbard model simulator.

Studying strong electron correlations has been an essential driving force for pushing the frontiers of condensed matter physics. In particular, in the vicinity of correlation-driven quantum phase transitions (QPTs), quantum critical fluctuations of multiple degrees of freedom facilitate exotic many-body states and quantum critical behaviours beyond Landau's framework1. Recently, moiré heterostructures of van der Waals materials have been demonstrated as highly tunable quantum platforms for exploring fascinating, strongly correlated quantum physics2-22. Here we report the observation of tunable quantum criticalities in an experimental simulator of the extended Hubbard model with spin-valley isospins arising in chiral-stacked twisted double bilayer graphene (cTDBG). Scaling analysis shows a quantum two-stage criticality manifesting two distinct quantum critical points as the generalized Wigner crystal transits to a Fermi liquid by varying the displacement field, suggesting the emergence of a critical intermediate phase. The quantum two-stage criticality evolves into a quantum pseudo criticality as a high parallel magnetic field is applied. In such a pseudo criticality, we find that the quantum critical scaling is only valid above a critical temperature, indicating a weak first-order QPT therein. Our results demonstrate a highly tunable solid-state simulator with intricate interplay of multiple degrees of freedom for exploring exotic quantum critical states and behaviours.

Approaching the Intrinsic Threshold Breakdown Voltage and Ultrahigh Gain in a Graphite/InSe Schottky Photodetector.

Realizing both ultralow breakdown voltage and ultrahigh gain is one of the major challenges in the development of high-performance avalanche photodetector. Here, it is reported that an ultrahigh avalanche gain of 3 × 105 can be realized in the graphite/InSe Schottky photodetector at a breakdown voltage down to 5.5 V. Remarkably, the threshold breakdown voltage can be further reduced down to 1.8 V by raising the operating temperature, approaching the theoretical limit of 1.5 E g \[{{\cal E}_{\bf g}}\] /e, with E g ${{\cal E}_{\bf g}}$ the bandgap of semiconductor. A 2D impact ionization model is developed and it is uncovered that observation of high gain at low breakdown voltage arises from reduced dimensionality of electron-phonon scattering in the layered InSe flake. These findings open up a promising avenue for developing novel weak-light detectors with low energy consumption and high sensitivity.

Nonvolatile van der Waals Heterostructure Phototransistor for Encrypted Optoelectronic Logic Circuit.

With the rising demand for information security, there has been a surge of interest in harnessing the intrinsic physical properties of device for designing a secure logic circuit. Here we provide an innovative approach to realize the secure optoelectronic logic circuit based on nonvolatile van der Waals (vdW) heterostructure phototransistors. The phototransistors comprising WSe2 and h-BN flakes exhibit electrical tunability of nonvolatile conductance under cooperative operations of electrical and light stimulus. This intriguing feature allows the phototransistor to work as a building block for the design of secure optoelectronic logic circuit in which the information encryption can be directly achieved with a designed secret key. On the basis of this approach, we assemble two phototransistors into an optoelectronic hybrid circuit and implement a functionally complete set of logic gates (i.e., NOR, XOR, and NAND) in a reconfigurable manner. Our findings highlight the potential of nonvolatile phototransistors for the development of reconfigurable secure optoelectronic circuits.

Networking retinomorphic sensor with memristive crossbar for brain-inspired visual perception.

Compared to human vision, conventional machine vision composed of an image sensor and processor suffers from high latency and large power consumption due to physically separated image sensing and processing. A neuromorphic vision system with brain-inspired visual perception provides a promising solution to the problem. Here we propose and demonstrate a prototype neuromorphic vision system by networking a retinomorphic sensor with a memristive crossbar. We fabricate the retinomorphic sensor by using WSe2/h-BN/Al2O3 van der Waals heterostructures with gate-tunable photoresponses, to closely mimic the human retinal capabilities in simultaneously sensing and processing images. We then network the sensor with a large-scale Pt/Ta/HfO2/Ta one-transistor-one-resistor (1T1R) memristive crossbar, which plays a similar role to the visual cortex in the human brain. The realized neuromorphic vision system allows for fast letter recognition and object tracking, indicating the capabilities of image sensing, processing and recognition in the full analog regime. Our work suggests that such a neuromorphic vision system may open up unprecedented opportunities in future visual perception applications.

Scalable massively parallel computing using continuous-time data representation in nanoscale crossbar array.

The growth of connected intelligent devices in the Internet of Things has created a pressing need for real-time processing and understanding of large volumes of analogue data. The difficulty in boosting the computing speed renders digital computing unable to meet the demand for processing analogue information that is intrinsically continuous in magnitude and time. By utilizing a continuous data representation in a nanoscale crossbar array, parallel computing can be implemented for the direct processing of analogue information in real time. Here, we propose a scalable massively parallel computing scheme by exploiting a continuous-time data representation and frequency multiplexing in a nanoscale crossbar array. This computing scheme enables the parallel reading of stored data and the one-shot operation of matrix-matrix multiplications in the crossbar array. Furthermore, we achieve the one-shot recognition of 16 letter images based on two physically interconnected crossbar arrays and demonstrate that the processing and modulation of analogue information can be simultaneously performed in a memristive crossbar array.

Observation of Negative Terahertz Photoconductivity in Large Area Type-II Dirac Semimetal PtTe_{2}.

As a newly emergent type-II Dirac semimetal, platinum telluride (PtTe_{2}) stands out from other two dimensional noble-transition-metal dichalcogenides for the unique band structure and novel physical properties, and has been studied extensively. However, the ultrafast response of low energy quasiparticle excitation in terahertz frequency remains nearly unexplored yet. Herein, we employ optical pump-terahertz probe (OPTP) spectroscopy to systematically study the photocarrier dynamics of PtTe_{2} thin films with varying pump fluence, temperature, and film thickness. Upon photoexcitation the terahertz photoconductivity (PC) of PtTe_{2} films shows abrupt increase initially, while the terahertz PC changes into negative value in a subpicosecond timescale, followed by a prolonged recovery process that lasted a few nanoseconds. The magnitude of both positive and negative terahertz PC response shows strongly pump fluence dependence. We assign the unusual negative terahertz PC to the formation of small polaron due to the strong electron-phonon (e-ph) coupling, which is further substantiated by temperature and film thickness dependent measurements. Moreover, our investigations give a subpicosecond timescale of simultaneous carrier cooling and polaron formation. The present study provides deep insights into the underlying dynamics evolution mechanisms of photocarrier in type-II Dirac semimetal upon photoexcitation, which is of crucial importance for designing PtTe_{2}-based optoelectronic devices.

Strain-Sensitive Magnetization Reversal of a van der Waals Magnet.

By virtue of the layered structure, van der Waals (vdW) magnets are sensitive to the lattice deformation controlled by the external strain, providing an ideal platform to explore the one-step magnetization reversal that is still conceptual in conventional magnets due to the limited strain-tuning range of the coercive field. In this study, a uniaxial tensile strain is applied to thin flakes of the vdW magnet Fe3 GeTe2 (FGT), and a dramatic increase of the coercive field (Hc ) by more than 150% with an applied strain of 0.32% is observed. Moreover, the change of the transition temperatures between the different magnetic phases under strain is investigated, and the phase diagram of FGT in the strain-temperature plane is obtained. Comparing the phase diagram with theoretical results, the strain-tunable magnetism is attributed to the sensitive change of magnetic anisotropy energy. Remarkably, strain allows an ultrasensitive magnetization reversal to be achieved, which may promote the development of novel straintronic device applications.

Tuning Electrical Conductance in Bilayer MoS2 through Defect-Mediated Interlayer Chemical Bonding.

Interlayer interaction could substantially affect the electrical transport in transition metal dichalcogenides, serving as an effective way to control the device performance. However, it is still challenging to utilize interlayer interaction in weakly interlayer-coupled materials such as pristine MoS2 to realize layer-dependent tunable transport behavior. Here, we demonstrate that, by substitutional doping of vanadium atoms in the Mo sites of the MoS2 lattice, the vanadium-doped monolayer MoS2 device exhibits an ambipolar field effect characteristic, while its bilayer device demonstrates a heavy p-type field effect feature, in sharp contrast to the pristine monolayer and bilayer MoS2 devices, both of which show similar n-type electrical transport behaviors. Moreover, the electrical conductance of the doped bilayer MoS2 device is drastically enhanced with respect to that of the doped monolayer MoS2 device. Employing first-principle calculations, we reveal that such striking behaviors arise from the presence of electrical transport networks associated with the enhanced interlayer hybridization of S-3pz orbitals between adjacent layers activated by vanadium dopants in the bilayer MoS2, which is nevertheless absent in its monolayer counterpart. Our work highlights that the effect of dopant not only is confined in the in-plane electrical transport behavior but also could be used to activate out-of-plane interaction between adjacent layers in tailoring the electrical transport of the bilayer transitional metal dichalcogenides, which may bring different applications in electronic and optoelectronic devices.

Gate-tunable van der Waals heterostructure for reconfigurable neural network vision sensor.

Early processing of visual information takes place in the human retina. Mimicking neurobiological structures and functionalities of the retina provides a promising pathway to achieving vision sensor with highly efficient image processing. Here, we demonstrate a prototype vision sensor that operates via the gate-tunable positive and negative photoresponses of the van der Waals (vdW) vertical heterostructures. The sensor emulates not only the neurobiological functionalities of bipolar cells and photoreceptors but also the unique connectivity between bipolar cells and photoreceptors. By tuning gate voltage for each pixel, we achieve reconfigurable vision sensor for simultaneous image sensing and processing. Furthermore, our prototype vision sensor itself can be trained to classify the input images by updating the gate voltages applied individually to each pixel in the sensor. Our work indicates that vdW vertical heterostructures offer a promising platform for the development of neural network vision sensor.

Van der Waals Heterostructures for High-Performance Device Applications: Challenges and Opportunities.

The discovery of two-dimensional (2D) materials with unique electronic, superior optoelectronic, or intrinsic magnetic order has triggered worldwide interest in the fields of material science, condensed matter physics, and device physics. Vertically stacking 2D materials with distinct electronic and optical as well as magnetic properties enables the creation of a large variety of van der Waals heterostructures. The diverse properties of the vertical heterostructures open unprecedented opportunities for various kinds of device applications, e.g., vertical field-effect transistors, ultrasensitive infrared photodetectors, spin-filtering devices, and so on, which are inaccessible in conventional material heterostructures. Here, the current status of vertical heterostructure device applications in vertical transistors, infrared photodetectors, and spintronic memory/transistors is reviewed. The relevant challenges for achieving high-performance devices are presented. An outlook into the future development of vertical heterostructure devices with integrated electronic and optoelectronic as well as spintronic functionalities is also provided.

Edge-Epitaxial Growth of InSe Nanowires toward High-Performance Photodetectors.

Semiconducting nanowires offer many opportunities for electronic and optoelectronic device applications due to their unique geometries and physical properties. However, it is challenging to synthesize semiconducting nanowires directly on a SiO2 /Si substrate due to lattice mismatch. Here, a catalysis-free approach is developed to achieve direct synthesis of long and straight InSe nanowires on SiO2 /Si substrates through edge-homoepitaxial growth. Parallel InSe nanowires are achieved further on SiO2 /Si substrates through controlling growth conditions. The underlying growth mechanism is attributed to a selenium self-driven vapor-liquid-solid process, which is distinct from the conventional metal-catalytic vapor-liquid-solid method widely used for growing Si and III-V nanowires. Furthermore, it is demonstrated that the as-grown InSe nanowire-based visible light photodetector simultaneously possesses an extraordinary photoresponsivity of 271 A W-1 , ultrahigh detectivity of 1.57 × 1014 Jones, and a fast response speed of microsecond scale. The excellent performance of the photodetector indicates that as-grown InSe nanowires are promising in future optoelectronic applications. More importantly, the proposed edge-homoepitaxial approach may open up a novel avenue for direct synthesis of semiconducting nanowire arrays on SiO2 /Si substrates.

Robust Impact-Ionization Field-Effect Transistor Based on Nanoscale Vertical Graphene/Black Phosphorus/Indium Selenide Heterostructures.

Maintaining the rapid development of information technology by scaling down a metal-oxide semiconductor field-effect transistor faces two serious challenges. First, the gate field loses control of the channel as it continuously decreases. Second, the fundamental thermionic limit restricts the reduction in supply voltage. Thus, further scaling down necessitates alternative device structures and different switching mechanisms. Here, we report impact-ionization transistors (IITs) based on nanoscale (∼30 nm) vertical graphene/black phosphorus (BP)/indium selenide (InSe) heterostructures. By facilitating the carrier multiplication of the ballistic impact-ionization process as the internal gain mechanism in sub-mean-free-path (sub-MFP) channels, the IITs exhibit a low average subthreshold swing (SS < 1 mV/dec) over five current levels. High stability (>10 000 cycles) and small hysteresis (<1%) switching properties are also obtained. The experimental demonstration of such transistor combining steep SS, high ON-state current density, reliable robustness, miniature footprint, and low bias voltage approaches fulfillments of targets for next-generation devices in the International Technology Roadmap for Semiconductors.

Direct Evidence for Charge Compensation-Induced Large Magnetoresistance in Thin WTe2.

Since the discovery of extremely large nonsaturating magnetoresistance (MR) in WTe2, much effort has been devoted to understanding the underlying mechanism, which is still under debate. Here, we explicitly identify the dominant physical origin of the large nonsaturating MR through in situ tuning of the magneto-transport properties in thin WTe2 film. With an electrostatic doping approach, we observed a nonmonotonic gate dependence of the MR. The MR reaches a maximum (10600%) in thin WTe2 film at certain gate voltage where electron and hole concentrations are balanced, indicating that the charge compensation is the dominant mechanism of the observed large MR. Besides, we show that the temperature-dependent magnetoresistance exhibits similar tendency with the carrier mobility when the charge compensation is retained, revealing that distinct scattering mechanisms may be at play for the temperature dependence of magneto-transport properties. Our work would be helpful for understanding mechanism of the large MR in other nonmagnetic materials and offers an avenue for achieving large MR in the nonmagnetic materials with electron-hole pockets.

Proximity-Induced Superconductivity with Subgap Anomaly in Type II Weyl Semi-Metal WTe2.

Due to the nontrivial topological band structure in type II Weyl semi-metal tungsten ditelluride (WTe2), unconventional properties may emerge in its superconducting phase. While realizing intrinsic superconductivity has been challenging in the type II Weyl semi-metal WTe2, the proximity effect may open an avenue for the realization of superconductivity. Here, we report the observation of proximity-induced superconductivity with a long coherence length along the c axis in WTe2 thin flakes based on a WTe2/NbSe2 van der Waals heterostructure. Interestingly, we also observe anomalous oscillations of the differential resistance during the transition from the superconducting to the normal state. Theoretical calculations show excellent agreement with experimental results, revealing that such a subgap anomaly is the intrinsic property of WTe2 in superconducting state induced by the proximity effect. Our findings enrich the understanding of the superconducting phase of type II Weyl semi-metals and pave the way for their future applications in topological quantum computing.

Experimental Identification of Critical Condition for Drastically Enhancing Thermoelectric Power Factor of Two-Dimensional Layered Materials.

Nanostructuring is an extremely promising path to high-performance thermoelectrics. Favorable improvements in thermal conductivity are attainable in many material systems, and theoretical work points to large improvements in electronic properties. However, realization of the electronic benefits in practical materials has been elusive experimentally. A key challenge is that experimental identification of the quantum confinement length, below which the thermoelectric power factor is significantly enhanced, remains elusive due to lack of simultaneous control of size and carrier density. Here we investigate gate-tunable and temperature-dependent thermoelectric transport in γ-phase indium selenide (γ-InSe, n-type semiconductor) samples with thickness varying from 7 to 29 nm. This allows us to properly map out dimension and doping space. Combining theoretical and experimental studies, we reveal that the sharper pre-edge of the conduction-band density of states arising from quantum confinement gives rise to an enhancement of the Seebeck coefficient and the power factor in the thinner InSe samples. Most importantly, we experimentally identify the role of the competition between quantum confinement length and thermal de Broglie wavelength in the enhancement of power factor. Our results provide an important and general experimental guideline for optimizing the power factor and improving the thermoelectric performance of two-dimensional layered semiconductors.