Two-Dimensional GeC/MXY (M = Zr, Hf; X, Y = S, Se) Heterojunctions Used as Highly Efficient Overall Water-Splitting Photocatalysts.

Hydrogen generation by photocatalytic water-splitting holds great promise for addressing the serious global energy and environmental crises, and has recently received significant attention from researchers. In this work, a method of assembling GeC/MXY (M = Zr, Hf; X, Y = S, Se) heterojunctions (HJs) by combining GeC and MXY monolayers (MLs) to construct direct Z-scheme photocatalytic systems is proposed. Based on first-principles calculations, we found that all the GeC/MXY HJs are stable van der Waals (vdW) HJs with indirect bandgaps. These HJs possess small bandgaps and exhibit strong light-absorption ability across a wide range. Furthermore, the built-in electric field (BIEF) around the heterointerface can accelerate photoinduced carrier separation. More interestingly, the suitable band edges of GeC/MXY HJs ensure sufficient kinetic potential to spontaneously accomplish water redox reactions under light irradiation. Overall, the strong light-harvesting ability, wide light-absorption range, small bandgaps, large heterointerfacial BIEFs, suitable band alignments, and carrier migration paths render GeC/MXY HJs highly efficient photocatalysts for overall water decomposition.

Designing edge states from fractional polarization insulators.

We theoretically investigated disconnected dispersive edge states in an anisotropic honeycomb lattice without chiral symmetry. When both mirror and chiral symmetries are present, this system is defined by a topological quantity known as fractional polarization (FP) term and exhibits a bulk band gap, classifying it as an FP insulator. While the FP insulator accommodates robust, flat topological edge states (TES), it also offers the potential to engineer these edge states by deliberately disrupting a critical symmetry that safeguards the underlying topology. These symmetry-breaking terms allow the edge states to become dispersive and generate differing configurations along the open boundaries. Furthermore, disconnected helical-like and chiral-like edge states analogous to TES seen in quantum spin and anomalous hall effect are achieved by the finite size effect, not possible from the symmetry-breaking terms alone. The demonstration of manipulating these edge states from a FP insulator can open up new avenues in constructing devices that utilize topological domain walls.

Nanoironing van der Waals Heterostructures toward Electrically Controlled Quantum Dots.

Assembling two-dimensional van der Waals (vdW)-layered materials into heterostructures is an exciting development that sparked the discovery of rich correlated electronic phenomena. vdW heterostructures also offer possibilities for designer device applications in areas such as optoelectronics, valley- and spintronics, and quantum technology. However, realizing the full potential of these heterostructures requires interfaces with exceptionally low disorder which is challenging to engineer. Here, we show that thermal scanning probes can be used to create pristine interfaces in vdW heterostructures. Our approach is compatible at both the material- and device levels, and monolayer WS2 transistors show up to an order of magnitude improvement in electrical performance from this technique. We also demonstrate vdW heterostructures with low interface disorder enabling the electrical formation and control of quantum dots that can be tuned from macroscopic current flow to the single-electron tunneling regime.

Experimental observation of exceptional bound states in a classical circuit network.

Exceptional bound (EB) states represent a unique new class of robust bound states protected by the defectiveness of non-Hermitian exceptional points. Conceptually distinct from the more well-known topological states and non-Hermitian skin states, they were recently discovered as a novel source of negative entanglement entropy in the quantum entanglement context. Yet, EB states have been physically elusive, being originally interpreted as negative probability eigenstates of the propagator of non-Hermitian Fermi gases. In this work, we show that EB states are in fact far more ubiquitous, also arising robustly in broad classes of systems whether classical or quantum. This hinges crucially on a newly-discovered spectral flow that rigorously justifies the EB nature of small candidate lattice systems. As a highlight, we present their first experimental realization through an electrical circuit, where they manifest as prominent stable resonant voltage profiles. Our work brings a hitherto elusive but fundamentally distinctive quantum phenomenon into the realm of classical metamaterials, and provides a novel pathway for the engineering of robust modes in otherwise sensitive systems..

Strongly correlated multielectron bunches from interaction with quantum light.

Strongly correlated electron systems are a cornerstone of modern physics, being responsible for groundbreaking phenomena from superconducting magnets to quantum computing. In most cases, correlations in electrons arise exclusively because of Coulomb interactions. In this work, we reveal that free electrons interacting simultaneously with a light field can become highly correlated via mechanisms beyond Coulomb interactions. In the case of two electrons, the resulting Pearson correlation coefficient for the joint probability distribution of the output electron energies is enhanced by more than 13 orders of magnitude compared to that of electrons interacting with the light field in succession (one after another). These highly correlated electrons are the result of momentum and energy exchange between the participating electrons via the external quantum light field. Our findings pave the way to the creation and control of highly correlated free electrons for applications including quantum information and ultrafast imaging.

Sub-5 nm Ultrathin In2O3 Transistors for High-Performance and Low-Power Electronic Applications.

Ultrathin oxide semiconductors are promising candidates for back-end-of-line (BEOL) compatible transistors and monolithic three-dimensional integration. Experimentally, ultrathin indium oxide (In2O3) field-effect transistors (FETs) with thicknesses down to 0.4 nm exhibit an extremely high drain current (104 µA/µm) and transconductance (4000 µS/µm). Here, we employ ab initio quantum transport simulation to investigate the performance limit of sub-5 nm gate length (Lg) ultrathin In2O3 FETs. Based on the International Technology Roadmap for Semiconductors (ITRS) criteria for high-performance (HP) devices, the scaling limit of ultrathin In2O3 FETs can reach 2 nm in terms of on-state current, delay time, and power dissipation. The wide bandgap nature of ultrathin In2O3 (3.0 eV) renders it a suitable candidate for ITRS low-power (LP) electronics with Lg down to 3 nm. Notably, both the HP and LP ultrathin In2O3 FETs exhibit superior energy-delay products as compared to those of other common 2D semiconductors such as monolayer MoS2 and MoTe2. These findings unveil the potential of ultrathin In2O3 in HP and LP nanoelectronic device applications.

Analytical Model of Optical-Field-Driven Subcycle Electron Tunneling Pulses from Two-Dimensional Materials.

We develop analytical models of optical-field-driven electron tunneling from the edge and surface of free-standing two-dimensional (2D) materials. We discover a universal scaling between the tunneling current density (J) and the electric field near the barrier (F): In(J/|F|ß) ∝ 1/|F| with ß values of 3/2 and 1 for edge emission and vertical surface emission, respectively. At ultrahigh values of F, the current density exhibits an unexpected high-field saturation effect due to the reduced dimensionality of the 2D material, which is absent in the traditional bulk material. Our calculation reveals the dc bias as an efficient method for modulating the optical-field tunneling subcycle emission characteristics. Importantly, our model is in excellent agreement with a recent experiment on graphene. Our results offer a useful framework for understanding optical-field tunneling emission from 2D materials, which are helpful for the development of optoelectronics and emerging petahertz vacuum nanoelectronics.

How to produce spin-splitting in antiferromagnetic materials.

Antiferromagnetic (AFM) materials have potential advantages for spintronics due to their robustness, ultrafast dynamics, and magnetotransport effects. However, the missing spontaneous polarization and magnetization hinders the efficient utilization of electronic spin in these AFM materials. Here, we propose a simple way to produce spin-splitting in AFM materials by making the magnetic atoms with opposite spin polarization locating in the different environment (surrounding atomic arrangement), which does not necessarily require the presence of spin-orbital coupling. We confirm our proposal by four different types of two-dimensional AFM materials within the first-principles calculations. Our works provide an intuitional design principle to find or produce spin-splitting in AFM materials.

Electric-field induced half-metallic properties in an experimentally synthesized CrSBr monolayer.

Two-dimensional (2D) half-metallic materials are highly desirable for nanoscale spintronic applications. Here, we propose a new mechanism that can achieve half-metallicity in 2D ferromagnetic (FM) materials with two-layer magnetic atoms by electric field tuning. We use a concrete example of an experimentally synthesized CrSBr monolayer to illustrate our proposal through first-principles calculations. It is found that half-metallic properties can be achieved in CrSBr within an appropriate electric field range, and the corresponding amplitude of electric field intensity can be realized experimentally. Janus monolayer Cr2S2BrI is constructed, which possesses a built-in electric field due to broken horizontal mirror symmetry. However, Cr2S2BrI without and with an applied external electric field is always a FM semiconductor. A possible memory device is also proposed based on the CrSBr monolayer. Our work will stimulate the application of 2D FM CrSBr in future spintronic nanodevices.

Single Atomic Defect Conductivity for Selective Dilute Impurity Imaging in 2D Semiconductors.

Precisely controlled impurity doping is of fundamental significance in modern semiconductor technologies. Desired physical properties are often achieved at impurity concentrations well below parts per million level. For emergent two-dimensional semiconductors, development of reliable doping strategies is hindered by the inherent difficulty in identifying and quantifying impurities in such a dilute limit where the absolute number of atoms to be detected is insufficient for common analytical techniques. Here we report rapid high-contrast imaging of dilute single atomic impurities by using conductive atomic force microscopy. We show that the local conductivity is enhanced by more than 100-fold by a single impurity atom due to resonance-assisted tunneling. Unlike the closely related scanning tunneling microscopy, the local conductivity sensitively depends on the impurity energy level, allowing minority defects to be selectively imaged. We further demonstrate subsurface impurity detection with single monolayer depth resolution in multilayer materials.

Janus monolayer ScXY (X≠Y = Cl, Br and I) for piezoelectric and valleytronic application: a first-principle prediction.

Coexistence of ferromagnetism, piezoelectricity and valley in two-dimensional (2D) materials is crucial to advance multifunctional electronic technologies. Here, Janus ScXY (X≠Y = Cl, Br and I) monolayers are predicted to be piezoelectric ferromagnetic semiconductors with dynamical, mechanical and thermal stabilities. They all show an in-plane easy axis of magnetization by calculating magnetic anisotropy energy (MAE) including magnetocrystalline anisotropy energy and magnetic shape anisotropy energy. The MAE results show that they intrinsically have no spontaneous valley polarization. The predicted piezoelectric strain coefficientsd11andd31(absolute values) are higher than ones of most 2D materials. Moreover, thed31(absolute value) of ScClI reaches up to 1.14 pm V-1, which is highly desirable for ultrathin piezoelectric device application. To obtain spontaneous valley polarization, charge doping are explored to tune the direction of magnetization of ScXY. By appropriate hole doping, their easy magnetization axis can change from in-plane to out-of-plane, resulting in spontaneous valley polarization. Taking ScBrI with 0.20 holes per f.u. as an example, under the action of an in-plane electric field, the hole carriers of K valley turn towards one edge of the sample, which will produce anomalous valley Hall effect, and the hole carriers of Γ valley move in a straight line. These findings could pave the way for designing piezoelectric and valleytronic devices.

Understanding Electronic Properties and Tunable Schottky Barriers in a Graphene/Boron Selenide van der Waals Heterostructure.

van der Waals heterostructures provide a powerful platform for engineering the electronic properties and for exploring exotic physical phenomena of two-dimensional materials. Here, we construct a graphene/BSe heterostructure and examine its electronic characteristics and the tunability of contact types under electric fields. Our results reveal that the graphene/BSe heterostructure is energetically, mechanically, and thermodynamically stable at room temperature. It forms a p-type Schottky contact and exhibits a high carrier mobility, making it a promising candidate for future Schottky field-effect transistors. Furthermore, applying an electric field not only reduces contact barriers but also induces a transition from a p-type to an n-type Schottky contact and from a Schottky to an ohmic contact, offering further potential for the control and manipulation of the heterostructure's electronic properties. Our findings offer a rational basis for the design of energy-efficient and tunable heterostructure devices based on the graphene/BSe heterostructure.

Liquid-Metal-Printed Ultrathin Oxides for Atomically Smooth 2D Material Heterostructures.

Two-dimensional (2D) semiconductors are promising channel materials for continued downscaling of complementary metal-oxide-semiconductor (CMOS) logic circuits. However, their full potential continues to be limited by a lack of scalable high-k dielectrics that can achieve atomically smooth interfaces, small equivalent oxide thicknesses (EOTs), excellent gate control, and low leakage currents. Here, large-area liquid-metal-printed ultrathin Ga2O3 dielectrics for 2D electronics and optoelectronics are reported. The atomically smooth Ga2O3/WS2 interfaces enabled by the conformal nature of liquid metal printing are directly visualized. Atomic layer deposition compatibility with high-k Ga2O3/HfO2 top-gate dielectric stacks on a chemical-vapor-deposition-grown monolayer WS2 is demonstrated, achieving EOTs of ∼1 nm and subthreshold swings down to 84.9 mV/dec. Gate leakage currents are well within requirements for ultrascaled low-power logic circuits. These results show that liquid-metal-printed oxides can bridge a crucial gap in dielectric integration of 2D materials for next-generation nanoelectronics.

Quantum Interference between Fundamentally Different Processes Is Enabled by Shaped Input Wavefunctions.

This work presents a general framework for quantum interference between processes that can involve different fundamental particles or quasi-particles. This framework shows that shaping input wavefunctions is a versatile and powerful tool for producing and controlling quantum interference between distinguishable pathways, beyond previously explored quantum interference between indistinguishable pathways. Two examples of quantum interference enabled by shaping in interactions between free electrons, bound electrons, and photons are presented: i) the vanishing of the zero-loss peak by destructive quantum interference when a shaped electron wavepacket couples to light, under conditions where the electron's zero-loss peak otherwise dominates; ii) quantum interference between free electron and atomic (bound electron) spontaneous emission processes, which can be significant even when the free electron and atom are far apart, breaking the common notion that a free electron and an atom must be close by to significantly affect each other's processes. Conclusions show that emerging quantum wave-shaping techniques unlock the door to greater versatility in light-matter interactions and other quantum processes in general.

Importance of magnetic shape anisotropy in determining magnetic and electronic properties of monolayer VSi2P4.

Two-dimensional (2D) ferromagnets have been a fascinating subject of research, and magnetic anisotropy (MA) is indispensable for stabilizing the 2D magnetic order. Here, we investigate magnetic anisotropy energy (MAE), magnetic and electronic properties ofVSi2P4by using the generalized gradient approximation plusUapproach. For largeU, the magnetic shape anisotropy (MSA) energy has a more pronounced contribution to the MAE, which can overcome the magnetocrystalline anisotropy (MCA) energy to evince an easy-plane. For fixed out-of-plane MA, monolayerVSi2P4undergoes ferrovalley (FV), half-valley-metal (HVM), valley-polarized quantum anomalous Hall insulator (VQAHI), HVM and FV states with increasingU. However, for assumptive in-plane MA, there is no special quantum anomalous Hall (QAH) state and spontaneous valley polarization within consideredUrange. According to the MAE and electronic structure with fixed out-of-plane or in-plane MA, the intrinsic phase diagram shows common magnetic semiconductor, FV and VQAHI in monolayerVSi2P4. At representativeU = 3 eV widely used in references,VSi2P4can be regarded as a 2D-XYmagnet, not Ising-like 2D long-range order magnets predicted in previous works with only considering MCA energy. Our findings shed light on importance of MSA in determining magnetic and electronic properties of monolayerVSi2P4.

MoSSe/Hf(Zr)S2 heterostructures used for efficient Z-scheme photocatalytic water-splitting.

Direct Z-scheme water-splitting is a promising route to enhancing the photocatalytic performance due to the effective separation of photogenerated carriers while simultaneously preserving the strong oxidation activity of holes and reduction activity of electrons. In this work, the MoSSe/XY2 (X = Hf, Zr; S, Se) heterostructures (HSs) with different contacts are proposed for Z-scheme photocatalytic water-spitting by first principles calculation. The separation of photogenerated carriers for HfSe2/SMoSe and ZrSe2/SMoSe HSs is limited by the type-I band alignment, while the hydrogen production ability of HfSe2/SeMoS and ZrSe2/SeMoS HSs is limited by the lower conduction band edge positions relative to the water reduction potential. The HfS2/SMoSe, HfS2/SeMoS, ZrS2/SMoSe, and ZrS2/SeMoS HSs are direct Z-scheme water-splitting photocatalysts with the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) occurring at the Hf(Zr)S2 layer and MoSSe layer, respectively. More excitingly, the S (or Se) vacancies effectively lower the HER overpotentials. Besides, the solar-to-hydrogen efficiencies are 6.1%, 5.9%, 6.4%, and 6.3% for HfS2/SMoSe, HfS2/SeMoS, ZrS2/SMoSe, and ZrS2/SeMoS HSs, respectively. This work paves the way for designing highly efficient overall water-splitting photocatalysts using 2D materials.

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.

Interface-Modulated Resistive Switching in Mo-Irradiated ReS2 for Neuromorphic Computing.

Coupling charge impurity scattering effects and charge-carrier modulation by doping can offer intriguing opportunities for atomic-level control of resistive switching (RS). Nonetheless, such effects have remained unexplored for memristive applications based on 2D materials. Here a facile approach is reported to transform an RS-inactive rhenium disulfide (ReS2 ) into an effective switching material through interfacial modulation induced by molybdenum-irradiation (Mo-i) doping. Using ReS2 as a model system, this study unveils a unique RS mechanism based on the formation/dissolution of metallic ß-ReO2 filament across the defective ReS2 interface during the set/reset process. Through simple interfacial modulation, ReS2 of various thicknesses are switchable by modulating the Mo-irradiation period. Besides, the Mo-irradiated ReS2 (Mo-ReS2 ) memristor further exhibits a bipolar non-volatile switching ratio of nearly two orders of magnitude, programmable multilevel resistance states, and long-term synaptic plasticity. Additionally, the fabricated device can achieve a high MNIST learning accuracy of 91% under a non-identical pulse train. The study's findings demonstrate the potential for modulating RS in RS-inactive 2D materials via the unique doping-induced charged impurity scattering property.

Two-dimensional penta-like PdPSe with a puckered pentagonal structure: a first-principles study.

Low-symmetry penta-PdPSe (Pd4P4Se4) with intrinsic in-plane anisotropy was synthesized successfully [P. Li et al., Adv. Mater., 2021, 2102541]. Motivated by this experimental discovery, we investigate the structural, mechanical, electronic, optical and thermoelectric properties of PdPSe nanosheets via density functional theory calculations. The phonon dispersion, molecular dynamics simulation, and cohesive energy mechanical properties of the penta-PdPSe are verified to confirm its stability. The phonon spectrum represents a striking gap between the high-frequency and the low-frequency optical branches and an out-of-plane flexure mode with a quadratic dispersion in the long-wavelength limit. The Poisson's ratio indicates that penta-PdPSe is a brittle nanosheet. The penta-PdPSe is a semiconductor with an indirect bandgap of 1.40 (2.07) eV using the PBE functional (HSE06 hybrid functional). Optical properties simulation suggests that PdPSe is capable of absorbing a substantial range of visible to ultraviolet light. Band alignment analysis also reveals the compatibility of PdPSe for water splitting photocatalysis application. By combining the electrical and thermal transport properties of PdPSe, we show that a high power factor is achievable at room temperature, thus making PdPSe a candidate material for thermoelectric applications. Our findings reveal the strong potential of penta-PdPSe nanosheets for a wide array of applications, including optoelectronic, water splitting and thermoelectric device applications.