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.

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.

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.

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.

Two-dimensional CdS/SnS2 heterostructure: a highly efficient direct Z-scheme water splitting photocatalyst.

A desired water splitting photocatalyst should not only possess a suitable bandgap and band edge position, but also host the spontaneous progress for overall water splitting without the aid of any sacrificial agents. In this work, we propose a two-dimensional CdS/SnS2 heterostructure (CSHS) as a possible water splitting photocatalyst by first-principles calculations. The CSHS enhances the absorption of visible and infrared light, and the type-II band alignment guarantees the spatial separation of the photoinduced carriers. The induced built-in electric field across the CSHS interface efficiently separates the photoexcited carriers and extends their carrier lifetimes. All these properties make the CSHS a direct Z-scheme system with the hydrogen and oxygen evolution reactions occurring, respectively, at the CdS and SnS2 layers. More encouragingly, the introduction of a S-vacancy into SnS2 could effectively lower the overpotential of the oxygen evolution reaction, thus ensuring the overall water redox reaction to be achieved spontaneously under light irradiation. Our findings suggest that the CSHS is a promising water splitting photocatalyst.

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.

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.

ZnSe Modified Zinc Metal Anodes: Toward Enhanced Zincophilicity and Ionic Diffusion.

Zinc metal is an ideal candidate for aqueous rechargeable batteries due to its high theoretical capacity and natural abundance. However, its commercialization is inevitably challenged by several critical factors such as dendrite growth and parasitic side-reactions, leading to low coulombic efficiency and a limited lifespan. Herein, a modified Zn foil with a zincophilic ZnSe layer deposited by a simple selenization process is proposed. An order of magnitude stronger adsorption capability toward Zn2+ ions and uniform ion diffusion tunnels of ZnSe enables lower nucleation energy barrier and faster ion-diffusion kinetics. Meanwhile, detrimental Zn corrosion in aqueous system is also effectively mitigated. As a result, ZnSe@Zn anode shows reversible Zn plating/stripping (1700 h at 1 mA cm-2 ) with ultra-low voltage hysteresis (41 mV), contributing to exceptional cycling stability over 500 cycles with negligible capacity fading for the ZnSe@Zn/MnO2 full cell.

Three-dimensional Dirac material anode enables concentrated solar thermionic converters.

Concentrated solar thermionic converters (CSTCs) are proposed by using three-dimensional (3D) Dirac material (DM) as the novel anode, significantly improving device performance. A theoretical model is developed to investigate the optimal performance of CSTCs. Under a solar concentration of 500, the CSTC reaches a maximum conversion efficiency of 11.8%. Furthermore, the optimal working condition and parametric selection criteria of the CSTC parameters under different solar concentrations are determined. Importantly, we demonstrate that 3D DM as an anode has more advantages over metal and graphene in CSTCs. This work thus offers a theoretical foundation for the exploration of solar thermionic application in using 3D DMs as novel electrodes.

Two-dimensional Dirac half-metal in porous carbon nitride C6N7monolayer via atomic doping.

Motivated by the recent experimental discovery of C6N7monolayer (Zhaoet al2021Science Bulletin66, 1764), we show that C6N7monolayer co-doped with C atom is a Dirac half-metal by employing first-principle density functional theory calculations. The structural, mechanical, electronic and magnetic properties of the co-doped C6N7are investigated by both the PBE and HSE06 functionals. Pristine C6N7monolayer is a semiconductor with almost isotropic electronic dispersion around the Γ point. As the doping of the C6N7takes place, the substitution of an N atom with a C atom transforms the monolayer into a dilute magnetic semiconductor, with the spin-up channel showing a band gap of 2.3 eV, while the spin-down channel exhibits a semimetallic phase with multiple Dirac points. The thermodynamic stability of the system is also checked out via AIMD simulations, showing the monolayer to be free of distortion at 500 K. The emergence of Dirac half-metal in carbon nitride monolayer via atomic doping reveals an exciting material platform for designing novel nanoelectronics and spintronics devices.

Designing high-performance nighttime thermoradiative systems for harvesting energy from outer space.

Energy harvesting using thermoradiative systems has been extensively explored in recent years as a novel strategy for further reducing our energy footprint. However, the nighttime application, thermodynamic limit, and optimal design of such a system remain largely unaddressed so far. Here we propose an improved nighttime thermoradiative system (NTS) for electrical power generation by optically coupling Earth's surface with outer space. Our theoretical model predicts that the NTS operating with Earth (deep space) at 300 K (3 K) yields a maximum power density of 12.3Wm-2 with an efficiency limit of 18.5%, which is potentially more advantageous than previous nighttime energy harvesting systems, such as a nighttime thermoelectric generator. We find that optimizing the thickness of the active layer, enhancing thermal infrared emission, and employing a silver backreflector for photon recycling are crucially important in improving system performance. This Letter provides new insights for the optimal designs of NTSs and paves the way toward practical nighttime power generation.

Design of an InSb thermoradiative system for harvesting low-grade waste heat.

We propose a thin-film InSb-based thermoradiative system (TRS) and assess its performance characteristics by using a parametric design at low-grade waste heat. We consider the effects of several loss mechanisms on system performance, including optical, sub-gap radiation, and non-radiative losses. Our results predict that the 50 nm thick InSb TRS operating with a hot (cold) source at 500 K (300 K) may yield a power density of 113 Wm-2 and an efficiency limit of 10.5%. To enhance the system performance, more efforts should be paid to optimize the layer thickness, enhance optical radiation, improve surface passivation, and fabricate an Ag back-reflective mirror and an optical filter for frequency-dependent photon recycling. This Letter provides new insights, to the best of our knowledge, for optimal designs and energy loss mechanisms, thus paving a route towards the development of practical TRS at a low temperature of around 500 K.

Universal Scaling Laws in Schottky Heterostructures Based on Two-Dimensional Materials.

We identify a new universality in the carrier transport of two-dimensional (2D) material-based Schottky heterostructures. We show that the reversed saturation current (J) scales universally with temperature (T) as log(J/T^{ß})∝-1/T, with ß=3/2 for lateral Schottky heterostructures and ß=1 for vertical Schottky heterostructures, over a wide range of 2D systems including nonrelativistic electron gas, Rashba spintronic systems, single- and few-layer graphene, transition metal dichalcogenides, and thin films of topological solids. Such universalities originate from the strong coupling between the thermionic process and the in-plane carrier dynamics. Our model resolves some of the conflicting results from prior works and is in agreement with recent experiments. The universal scaling laws signal the breakdown of ß=2 scaling in the classic diode equation widely used over the past sixty years. Our findings shall provide a simple analytical scaling for the extraction of the Schottky barrier height in 2D material-based heterostructures, thus paving the way for both a fundamental understanding of nanoscale interface physics and applied device engineering.

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.

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.

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.

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.