Search

Future electronics require aggressive scaling of channel material thickness while maintaining device performance. Two-dimensional (2D) semiconductors are promising candidates, but despite over two decades of research, experimental performance still lags theoretical expectations. Here, we develop an oxygen-free approach to push the electrical transport of 2D field-effect transistors toward the theoretical phonon-limited intrinsic mobility. We achieve record carrier mobilities of 91 (132) cm2V-1s-1 for mono- (bi-) layer MoS2 transistors on SiO2 substrate. Statistics from over 60 devices confirm that oxygen-free fabrication enhances key figures of merit by more than an order of magnitude. While previous studies suggest that 2D transition metal dichalcogenides such as MoS2 and WS2 are stable in air, we show that short-term ambient exposure can degrade their device performance through irreversible oxygen chemisorption. This study emphasizes the criticality of avoiding oxygen exposure, offering guidance for device manufacturing for fundamental research and practical applications of 2D materials.

Ultrathin oxide semiconductors with sub-1-nm thickness are promising building blocks for ultrascaled field-effect transistor (FET) applications due to their resilience against short-channel effects, high air stability, and potential for low-energy device operation. However, the n-type dominance of ultrathin oxide FET has hindered their integration into complementary metal-oxide-semiconductor (CMOS) technology, which requires both n-and p-type devices. Here we develop an ab initio device-driven computational screening workflow to identify sub-1-nm thickness oxide semiconductors for sub-5-nm FET applications. We demonstrate that ultrathin CaO2, CaO, and SrO are compatible with p-type device operations under both high-performance (HP) and low-power (LP) requirements specified by the International Technology Roadmap of Semiconductors (ITRS), thereby expanding the limited family of p-type oxide semiconductors. Notably, CaO and SrO emerge as the first-of-kind sub-1-nm thickness oxide semiconductors capable of simultaneously meeting the ITRS HP and LP criteria for both n-and p-type devices. CaO and SrO FETs outperform many existing low-dimensional semiconductors, exhibiting scalability below 5-nm gate length. Our findings offer a pioneering effort in the ab initio, device-driven screening of sub-1-nm thickness oxide semiconductors, significantly broadening the material candidate pool for future CMOS technology nodes., Comment: 23 pages, 5 figures, 1 table

Electrical manipulation of spin-polarized current is highly desirable yet tremendously challenging in developing ultracompact spintronic device technology. Here we propose a scheme to realize the all-electrical manipulation of spin-polarized current in an altermagnetic bilayer. Such a bilayer system can host layer-spin locking, in which one layer hosts a spin-polarized current while the other layer hosts a current with opposite spin polarization. An out-of-plane electric field breaks the layer degeneracy, leading to a gate-tunable spin-polarized current whose polarization can be fully reversed upon flipping the polarity of the electric field. Using first-principles calculations, we show that CrS bilayer with C-type antiferromagnetic exchange interaction exhibits a hidden layer-spin locking mechanism that enables the spin polarization of the transport current to be electrically manipulated via the layer degree of freedom. We demonstrate that sign-reversible spin polarization as high as 87% can be achieved at room temperature. This work presents the pioneering concept of layer-spintronics which synergizes altermagnetism and bilayer stacking to achieve efficient electrical control of spin., Comment: 20 pages, 5 figures

Wide bandgap oxide semiconductors are very promising channel candidates for next-generation electronics due to their large-area manufacturing, high-quality dielectrics, low contact resistance, and low leakage current. However, the absence of ultra-short gate length (Lg) p-type transistors has restricted their application in future complementary metal-oxide-semiconductor (CMOS) integration. Inspired by the successfully grown high-hole mobility bilayer (BL) beta tellurium dioxide (\b{eta}-TeO2), we investigate the performance of sub-5-nm-Lg BL \b{eta}-TeO2 field-effect transistors (FETs) by utilizing first-principles quantum transport simulation. The distinctive anisotropy of BL \b{eta}-TeO2 yields different transport properties. In the y-direction, both the sub-5-nm-Lg n-type and p-type BL \b{eta}-TeO2 FETs can fulfill the International Technology Roadmap for Semiconductors (ITRS) criteria for high-performance (HP) devices, which are superior to the reported oxide FETs (only n-type). Remarkably, we for the first time demonstrate the existence of the NMOS and PMOS symmetry in sub-5-nm-Lg oxide semiconductor FETs. As to the x-direction, the n-type BL \b{eta}-TeO2 FETs satisfy both the ITRS HP and low-power (LP) requirements with Lg down to 3 nm. Consequently, our work shed light on the tremendous prospects of BL \b{eta}-TeO2 for CMOS application.

Graphene nanoribbon (GNR) emerges as an exceptionally promising channel candidate due to its tunable sizable bandgap (0-3 eV), ultrahigh carrier mobility (up to 4600 cm^(2) V^(-1) s^(-1)), and excellent device performance (current on-off ratio of 10^(7)). However, the asymmetry of reported n-type and p-type GNR field-effect transistors (FETs) at ultrashort gate length (Lg) has become an obstacle to future complementary metal-oxide-semiconductor (CMOS) integration. Here, we conduct ab initio quantum transport simulations to investigate the transport properties of sub-5-nm Lg 7 armchair-edge GNR (7 AGNR) FETs. The on-state current, delay time, and power dissipation of the n-type and p-type 7 AGNR FETs fulfill the International Technology Roadmap for Semiconductors targets for high-performance devices when Lg is reduced to 3 nm. Remarkably, the 7 AGNR FETs exhibit superior n-type and p-type symmetry to the 7-9-7 AGNR FETs due to the more symmetrical electron/hole effective masses. Compared to the monolayer MoS2 and MoTe2 counterparts, the 7 AGNR FETs have better device performance, which could be further improved via gate engineering. Our results shed light on the immense potential of 7 AGNR in advancing CMOS electronics beyond silicon.

The Kane-Mele model has been modified to achieve versatile topological phases. Previous work [Phys. Rev. Lett. 120, 156402 (2018)] introduced a staggered intrinsic spin-orbit coupling effect to generate pseudohelical edge states, with Rashba spin-orbit coupling facilitating spin flips in alternating sublattices. Our study demonstrates that, in the absence of Rashba spin-orbit coupling, the modified Kane-Mele model with staggered intrinsic spin-orbit coupling evolves into a $Z_{2}$ class topological metal, specifically a two-dimensional Weyl nodal-line semimetal. In a nanoribbon geometry, we predict the emergence of antihelical edge states, which support spin-polarized currents flowing in the same direction along parallel boundaries. Unlike pseudohelical edge states, antihelical edge states can be viewed as a superposition of two antichiral edge states related by time-reversal symmetry. However, the spin Hall conductance from antihelical edge states is not quantized due to the presence of gapless bulk states. Additionally, we examine the robustness of helical, pseudohelical, and antihelical edge states in the presence of nonmagnetic disorders, highlighting the particular fragility of antihelical edge states. Our findings enhance the understanding of the modified Kane-Mele model, providing new insights into its topological properties., Comment: 10 pages, 8 figures

Floquet engineering of topological phase transitions driven by a high-frequency time-periodic field is a promising approach to realizing new topological phases of matter distinct from static states. Here, we theoretically investigate Floquet engineering topological phase transitions in the quantum spin Hall $\alpha$-$T_{3}$ system driven by an off-resonant circularly polarized light. In addition to the quantum spin (anomalous) Hall insulator phase with multiple helical (chiral) edge states, spin-polarized topological metallic phases are observed, where the bulk topological band gap of one spin sub-band overlaps with the other gapless spin sub-band. Moreover, with a staggered potential, the topological invariants of the system depend on whether the middle band is occupied because of the breaking of particle-hole symmetry. Our work highlights the significance of Floquet engineering in realizing new topological phases in $\alpha$-$T_{3}$ lattices., Comment: 11 pages, 6 figures

Using first-principles simulations combined with many-body calculations, we show that two-dimensional free-standing quintuple-layer Bi2Se2Te is an inversion symmetric monolayer expected to achieve spatially indirect exciton with large exciton radius, small exciton effective mass and long exciton lifetime. Such system is theoretically predicted to be a promising platform for realizing excitonic Bose-Einstein condensation and superfluid due to its high phase transition temperatures of ~257 K and ~64.25 K for the BEC and excitonic superfluid, respectively. The importance of spin-orbit coupling is revealed, and the angular momentum selection rules for photon absorption are discussed. This finding suggests the potential of QL Bi2Se2Te monolayer with exotic bosonic bound states provides as a tantalizing high-temperature platform to probe excitonic physics.

Non-reciprocal devices are key components in modern electronics covering broad applications ranging from transistors to logic circuits thanks to the output rectified signal in the direction parallel to the input. In this work, we propose a transverse Cooper-pair rectifier in which a non-reciprocal current is perpendicular to the driving field, when inversion, time reversal, and mirror symmetries are broken simultaneously. The Blonder-Tinkham-Klapwijk formalism is developed to describe the transverse current-voltage relation in a normal-metal/superconductor tunneling junction, where symmetry constraints are achieved by an effective built-in supercurrent manifesting in an asymmetric and anisotropic Andreev reflection. The asymmetry in the Andreev reflection is induced when inversion and time reversal symmetry are broken by the supercurrent component parallel to the junction while the anisotropy occurs when the mirror symmetry with respect to the normal of the junction interface is broken by the perpendicular supercurrent component to the junction. Compared to the conventional longitudinal one, the transverse rectifier supports fully polarized diode efficiency and colossal nonreciprocal conductance rectification, completely decoupling the path of the input excitation from the output rectified signal. This work provides a formalism for realizing transverse non-reciprocity in superconducting junctions, which is expected to be achieved by modifying current experimental setups and may pave the way for future low-dissipation superconducting electronics., Comment: 9 + 13 pages, 3 + 6 figures

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 due to 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 (PCC) for the joint probability distribution of the output electron energies is enhanced over 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 ultra-fast imaging., Comment: 3 figures for Main Text, 4 figures for Supplementary Materials, Supplementary is available at end of Main Text figures

Assembling two-dimensional van der Waals layered materials into heterostructures is an exciting development that sparked the discovery of rich correlated electronic phenomena and offers possibilities for designer device applications. However, resist residue from fabrication processes is a major limitation. Resulting disordered interfaces degrade device performance and mask underlying transport physics. Conventional cleaning processes are inefficient and can cause material and device damage. Here, we show that thermal scanning probe based cleaning can effectively eliminate resist residue to recover pristine material surfaces. Our technique is compatible at both the material- and device-level, and we demonstrate the significant improvement in the electrical performance of 2D WS2 transistors. We also demonstrate the cleaning of van der Waals heterostructures to achieve interfaces with low disorder. This enables the electrical formation and control of quantum dots that can be tuned from macroscopic current flow to the single-electron tunnelling regime. Such material processing advances are crucial for constructing high-quality vdW heterostructures that are important platforms for fundamental studies and building blocks for quantum and nano-electronics applications., Comment: 4 Figures

The combination of antiferromagnetic (AFM) spintronics and anomalous valley Hall effect (AVHE) is of great significance for potential applications in valleytronics. Here, we propose a design principle for achieving AVHE in A-type hexagonal AFM monolayer. The design principle involves the introduction of layer-dependent electrostatic potential caused by out-of-plane external electric field, which can break the combined symmetry ($PT$ symmetry) of spatial inversion ($P$) and time reversal ($T$), producing spin splitting. The spin order of spin splitting can be reversed by regulating the direction of electric field. Based on first-principles calculations, the design principle can be verified in AFM $\mathrm{Cr_2CH_2}$. The layer-locked hidden Berry curvature can give rise to layer-Hall effect, including valley layer-spin Hall effect and layer-locked AVHE. Our works provide an experimentally feasible way to realize AVHE in AFM monolayer., Comment: 5 pages,6 figures

We study the topological properties of the Haldane and modified Haldane models in $\alpha$-$T_{3}$ lattice. The band structures and phase diagrams of the system are investigated. Individually, each model undergoes a distinct phase transition: (i) the Haldane-only model experiences a topological phase transition from the Chern insulator ($\mathcal{C} = 1$) phase to the higher Chern insulator ($\mathcal{C} = 2$) phase; while (ii) the modified-Haldane-only model experiences a phase transition from the topological metal ($\mathcal{C} = 2$) phase to the higher Chern insulator ($\mathcal{C} = 2$) phase and we show that $\mathcal{C}$ is insufficient to characterize this system because $\mathcal{C}$ remains unchanged before and after the phase transition. By plotting the Chern number and $\mathcal{C}$ phase diagram, we show that in the presence of both Haldane and modified Haldane models in the $\alpha$-$T_{3}$ lattice, the interplay between the two models manifests three distinct topological phases, namely the $\mathcal{C} = 1$ Chern insulator (CI) phase, $\mathcal{C} = 2$ higher Chern insulator (HCI) phase and $\mathcal{C} = 2$ topological metal (TM) phase. These results are further supported by the $\alpha$-$T_{3}$ zigzag edge states calculations. Our work elucidates the rich phase evolution of Haldane and modified Haldane models as $\alpha$ varies continuously from $0$ to $1$ in an $\alpha$-$T_3$ model., Comment: 9 pages, 5 figures

Antiferromagnetic (AFM) spintronics provides a route towards energy-efficient and ultrafast device applications. Achieving anomalous valley Hall effect (AVHE) in AFM monolayers is thus of considerable interest for both fundamental condensed matter physics and device enginering. Here we propose a route to achieve AVHE in A-type AFM insulator composed of vertically-stacked monolayer quantum anomalous Hall insulator (QAHI) with strain and electric field modulations. Uniaxial strain and electric field generate valley polarization and spin splitting, respectively. Using first-principles calculations, $\mathrm{Fe_2BrMgP}$ monolayer is predicted to be a prototype A-type AFM hosting \emph{valley-polarized quantum spin Hall insulator} (VQSHI) in which AVHE and quantum spin Hall effect (QSHE) are synergized in a single system. Our findings reveal a route to achieve multiple Hall effects in 2D tetragonal AFM monolayers., Comment: 6 pages, 6 figures

Recent discovery of ultrathick $\mathrm{MoSi_2N_4(MoN)_n}$ monolayers open up an exciting platform to engineer 2D material properties via intercalation architecture. Here we computationally investigate a series of ultrathick MA$_2$N$_4$(M'N) monolayers (M, M' = Mo, W; A = Si, Ge) under both homolayer and heterolayer intercalation architectures in which the same and different species of transition metal nitride inner core layers are intercalated by outer passivating nitride sublayers, respectively. The MA$_2$N$_4$(M'N) monolayers are thermally, dynamically and mechanically stable with excellent mechanical strength and metallic properties. Intriguingly, the metallic states around Fermi level are localized within the inner core layers. Carrier conduction mediated by electronic states around the Fermi level is thus spatially insulated from the external environment by the native outer nitride sublayers, suggesting the potential of MA$_2$N$_4$(M'N) in back-end-of-line (BEOL) metal interconnect applications. Nitrogen vacancy defect at the outer sublayers creates `punch through' states around the Fermi level that bridges the carrier conduction in the inner core layers and the outer environment, forming a electrical contact akin to the `vias' structures of metal interconnects. We further show that MoSi$_2$N$_4$(MoN) can serve as a quasi-Ohmic contact to 2D WSe$_2$. These findings reveal the promising potential of ultrathick MA$_2$N$_4$(MN) monolayers as metal electrodes and BEOL interconnect applications., Comment: 13 pages, 7 figures, 3 tables

Ultra-thin (UT) oxide semiconductors are promising candidates for back-end-of-line (BEOL) compatible transistors and monolithic three-dimensional integration. Experimentally, UT indium oxide (In$_2$O$_3$) field-effect transistors (FETs) with thicknesses down to 0.4 nm exhibits extremely high drain current (10000 $\mu$A/$\mu$m) and transconductance (4000 $\mu$S/$\mu$m). Here, we employ the ab initio quantum transport simulation to investigate the performance limit of sub-5-nm gate length (Lg) UT In$_2$O$_3$ FET. Based on the International Technology Roadmap for Semiconductors (ITRS) criteria for high-performance (HP) devices, the scaling limit of UT In$_2$O$_3$ FETs can reach 2 nm in terms of on-state current, delay time, and power dissipation. The wide bandgap nature of UT In$_2$O$_3$ (3.15 eV) renders it a suitable candidate for ITRS low-power (LP) electronics with Lg down to 3 nm. Both the HP and LP UT In$_2$O$_3$ FETs exhibit superior energy-delay products as compared to other common 2D semiconductors such as monolayer MoS2 and MoTe2. Our study unveils the immense promise of UT In$_2$O$_3$ for both HP and LP device applications., Comment: 16 pages, 7 figures

Exceptional points are complex branching singularities of non-Hermitian bands that have lately attracted considerable interest, particularly in non-Hermitian photonics. In this article, we review some recent developments in non-Hermitian photonic platforms such as waveguides, photonic crystals, Fabry-Perot resonators and plasmonic systems, and suggest how optical non-linearities and exceptional bound states can significantly impact the development of non-Hermitian photonics in the near future.

Altermagnet is an emerging antiferromagnetic material subclass that exhibits spin-splitting in momentum space without net global magnetization and spin-orbit-coupling effect. In this work, we develop a model of thermal charge injection across an altermagnet/semiconductor (AM/S) Schottky contact. We obtain analytical expressions describing the spin-dependent thermionic current injection across the AM/S contact under any arbitrary interface orientation angles. Interestingly, the spin-contrasting Fermi surface of an altermagnetic electrode enables spin-polarized current to be injected into a nonmagnetic semiconductor even though the system has net-zero magnetization. Our findings thus reveal an altermagntic mechanism to achieve spin injection without involving ferromagnetic ordering. The AM/S Schottky contact proposed here shall provide a potential altermagnetic building block of spintronic devices that are resilient against stray magnetic field perturbation and inherently compatible with ultracompact integration., Comment: 8 pages, 3 figures

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 (SOC). We confirm our proposal by four different types of two-dimensional (2D) AFM materials within the first-principles calculations. Our works provide a intuitional design principle to find or produce spin-splitting in AFM materials., Comment: 6 pages, 9 figures

Gate-all-around (GAA) nanowire (NW) field-effect transistor (FET) is a promising device architecture due to its superior gate controllability than that of the conventional FinFET architecture. The significantly higher electron mobility of indium phosphide (InP) NW than silicon NW makes it particularly well-suited for high-performance (HP) electronics applications. In this work, we perform an ab initio quantum transport simulation to investigate the performance limit of sub-5-nm gate length (Lg) GAA InP NW FETs. The GAA InP NW FETs with Lg of 4 nm can meet the International Technology Roadmap for Semiconductors (ITRS) requirements for HP devices from the perspective of on-state current, delay time, and power dissipation. We also investigate the impact of strain on 3-nm-Lg GAA InP NW FETs. The application of tensile strain results in a remarkable increase of over 60% in the on-state current. These results highlight the potential of GAA InP NW FETs for HP applications in the sub-5-nm Lg region., Comment: 22 pages, 7 figures

Two-dimensional (2D) ferrovalley semiconductor (FVSC) with spontaneous valley polarization offers an exciting material platform for probing Berry phase physics. How FVSC can be incorporated in valleytronic device applications, however, remain an open question. Here we generalize the concept of metal/semiconductor (MS) contact into the realm of valleytronics. We propose a half-valley Ohmic contact based on FVSC/graphene heterostructure where the two valleys of FVSC separately forms Ohmic and Schottky contacts with those of graphene, thus allowing current to be valley-selectively injected through the `Ohmic' valley while being blocked in the `Schottky' valley. We develop a theory of contact-limited valley-contrasting current injection and demonstrate that such transport mechanism can produce gate-tunable valley-polarized injection current. Using RuCl$_2$/graphene heterostructure as an example, we illustrate a device concept of valleytronic barristor where high valley polarization efficiency and sizable current on/off ratio, can be achieved under experimentally feasible electrostatic gating conditions. These findings uncover contact-limited valley-contrasting current injection as an efficient mechanism for valley polarization manipulation, and reveals the potential of valleytronic MS contact as a functional building block of valleytronic device technology., Comment: 9 pages, 5 figures

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) material with two-layer magnetic atoms by electric field tuning. We use a concrete example of experimentally synthesized CrSBr monolayer to illustrate our proposal through the first-principle calculations. It is found that the half-metal can be achieved in CrSBr within appropriate electric field range, and the corresponding amplitude of electric field intensity is available in experiment. Janus monolayer $\mathrm{Cr_2S_2BrI}$ is constructed, which possesses built-in electric field due to broken horizontal mirror symmetry. However, $\mathrm{Cr_2S_2BrI}$ without and with applied external electric field is always a FM semiconductor. A possible memory device is also proposed based on CrSBr monolayer. Our works will stimulate the application of 2D FM CrSBr in future spintronic nanodevices., Comment: 6 pages, 7 figures

Exceptional bound (EB) states represent an 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., Comment: 14 pages, 8 figures

Carrier conduction in wide bandgap semiconductors (WBS) often exhibits velocity saturation at the high-electric field regime. How such effect influences the transition between contact-limited and space-charge-limited current in a two-terminal device remains largely unexplored thus far. Here, we develop a generalized carrier transport model that includes contact-limited field-induced carrier injection, space charge, carrier scattering and velocity saturation effect. The model reveals various transitional behaviors in the current-voltage characteristics, encompassing Fowler-Nordheim emission, trap-free Mott-Gurney (MG) SCLC and \emph{velocity-saturated SCLC}. Using GaN, 6H-SiC and 4H-SiC WBS as examples, we show that the velocity-saturated SCLC completely dominates the high-voltage ($10^2 \sim 10^4$ V) transport for typical sub-$\mu$m GaN and SiC diodes, thus unravelling velocity-saturated SCLC as a central transport mechanism in WBG electronics., Comment: 8 pages, 5 figures

We develop a theoretical model to calculate the quantum efficiency (QE) of photoelectron emission from materials with Rashba spin-orbit coupling (RSOC) effect. In the low temperature limit, an analytical scaling between QE and the RSOC strength is obtained as QE $\propto (\hbar\omega-W)^2+2E_R(\hbar \omega-W) -E_R^2/3$, where $\hbar\omega$, $W$ and $E_R$ are the incident photon energy, work function and the RSOC parameter respectively. Intriguingly, the RSOC effect substantially improves the QE for strong RSOC materials. For example, the QE of Bi$_2$Se$_3$ and Bi/Si(111) increases, by 149\% and 122\%, respectively due to the presence of strong RSOC. By fitting to the photoelectron emission characteristics, the analytical scaling law can be employed to extract the RSOC strength, thus offering a useful tool to characterize the RSOC effect in materials. Importantly, when the traditional Fowler-Dubridge model is used, the extracted results may substantially deviate from the actual values by $\sim90\%$, thus highlighting the importance of employing our model to analyse the photoelectron emission especially for materials with strong RSOC. These findings provide a theoretical foundation for the design of photoemitters using Rashba spintronic materials., Comment: 6 pages, 3 figures

The sustainable development of next-generation device technology is paramount in the face of climate change and the looming energy crisis. Tremendous efforts have been made in the discovery and design of nanomaterials that achieve device-level sustainability, where high performance and low operational energy cost are prioritized. However, many of such materials are composed of elements that are under threat of depletion and pose elevated risks to the environment. The role of material-level sustainability in computational screening efforts remains an open question thus far. Here we develop a general van der Waals materials screening framework imbued with sustainability-motivated search criteria. Using ultrawide bandgap (UWBG) materials as a backdrop -- an emerging materials class with great prospects in dielectric, power electronics, and ultraviolet device applications, we demonstrate how this screening framework results in 25 sustainable UWBG layered materials comprising only of low-risks elements. Our findings constitute a critical first-step towards reinventing a more sustainable electronics landscape beyond silicon, with the framework established in this work serving as a harbinger of sustainable 2D materials discovery., Comment: 17 pages, 8 figures

We theoretically investigated the topological-protected edge states (TESs) in an anisotropic honeycomb lattice with mirror and chiral symmetries, characterized by an alternative topological invariant - fractional polarization (FP), rather than the conventional Chern number. This system termed an FP insulator is a potential platform for edge-state engineering due to its disconnected TESs. These disconnected and robust TESs are susceptible to perturbative chiral symmetry-breaking terms which can generate various patterns including the vanishing helical, spin-polarized, and chiral TESs. Moreover, helical and chiral TES can be achieved by the finite size effect, not possible from the aforementioned terms alone. The demonstration of these various TES in an FP-insulator offers an alternative route in designing reconfigurable two-dimensional nanoelectronic devices., Comment: 9 pages, 4 figures

The altermagnetism can achieve spin-split bands in collinear symmetry-compensated antiferromagnets. Here, we predict altermagnetic order in Janus monolayer $\mathrm{Cr_2SO}$ with eliminated inversion symmetry, which can realize the combination of piezoelectricity and altermagnetism in a two-dimensional material, namely 2D piezoelectric altermagnetism. It is found that $\mathrm{Cr_2SO}$ is an altermagnetic semiconductor, and the spin-split bands of both valence and conduction bands are near the Fermi level. The $\mathrm{Cr_2SO}$ has large out-of-plane piezoelectricity ($|d_{31}|$$=$0.97 pm/V), which is highly desirable for ultrathin piezoelectric device application. Due to spin-valley locking, both spin and valley can be polarized by simply breaking the corresponding crystal symmetry with uniaxial strain. Our findings provide a platform to integrate spin, piezoelectricity and valley in a single material, which is useful for multi-functional device applications., Comment: 6 pages, 5 figures

The persistent spin helix (PSH) is robust against spin-independent scattering and renders an extremely long spin lifetime, which can improve the performance of potential spintronic devices. To achieve the PSH, a unidirectional spin configuration is required in the momentum space. Here, T-XY (X$\neq$Y=P, As, Sb and Bi) monolayers with dynamical, mechanical and thermal stabilities are predicted to intrinsically possess PSH. Due to the $C_{2\upsilon}$ point-group symmetry, a unidirectional spin configuration is preserved in the out-of-plane direction for both conduction and valence bands around the high-symmetry $\Gamma$ point. That is, the expectation value of the spin $S$ only has the out-of-plane component $S_z$. The application of an out-of-plane external electric field can induce in-plane components $S_x$ and $S_y$, thus offering a promising platform for the on-off logical functionality of spin devices. Our work reveals a new family of T-phase two-dimensional (2D) materials, which could provide promising applications in spintronic devices., Comment: 7 pages, 7 figures

Recent experimental synthesis of ambient-stable MoSi2N4 monolayer have garnered enormous research interests. The intercalation morphology of MoSi2N4 - composed of a transition metal nitride (Mo-N) inner sub-monolayer sandwiched by two silicon nitride (Si-N) outer sub-monolayers - have motivated the computational discovery of an expansive family of synthetic MA2Z4 monolayers with no bulk (3D) material counterpart (where M = transition metals or alkaline earth metals; A = Si, Ge; and N = N, P, As). MA2Z4 monolayers exhibit interesting electronic, magnetic, optical, spintronic, valleytronic and topological properties, making them a compelling material platform for next-generation device technologies. Furthermore, heterostructure engineering enormously expands the opportunities of MA2Z4. In this review, we summarize the recent rapid progress in the computational design of MA2Z4-based heterostructures based on first-principle density functional theory (DFT) simulations - a central \emph{work horse} widely used to understand the physics, chemistry and general design rules for specific targeted functions. We systematically classify the MA2Z4-based heterostructures based on their contact types, and review their physical properties, with a focus on their performances in electronics, optoelectronics and energy conversion applications. We review the performance and promises of MA2Z4-based heterostructures for device applications that include electrical contacts, transistors, spintronic devices, photodetectors, solar cells, and photocatalytic water splitting. This review unveils the vast device application potential of MA2Z4-based heterostructures, and paves a roadmap for the future experimental and theoretical development of MA2Z4-based functional heterostructures and devices., Comment: 32 pages, 15 figures

We develop analytical models of optical-field electron tunneling from the edge and surface of two-dimensional (2D) materials, including the effects of reduced dimensionality, non-parabolic energy dispersion, band anisotropy, quasi-time dependent tunneling and emission dynamics indueced by the laser field. We discover a universal scaling between the tunneling current density $J$ and the laser electric field $F$: In($J/|F|^{\beta})\propto1/|F|$ with $\beta = 3 / 2$ in the edge emission and $\beta = 1$ in the vertical surface emission, which both are distinctive from the traditional Fowler-Nordheim (FN) model of $\beta = 2$. The current density exhibits an unexpected high-field saturation effect due to the reduced dimensionality of 2D materials, which is completely different from the space-charge saturation commonly observed in traditional bulk materials. Our results reveal the dc bias as an efficient method in modulating the optical-field tunneling sub-optical-cycle emission characteristics. Importantly, our model is in excellent agreement with a recent experiment on graphene. Our findings offer a theoretical foundation for the understanding of optical-field tunneling emission from the 2D material system, which is useful for the development of 2D-material based optoelectronics and vacuum nanoelectronics., Comment: 8 pages, 2 figures, 2 tables

Coexistence of ferromagnetism, piezoelectricity and valley in two-dimensional (2D) materials is crucial to advance multifunctional electronic technologies. Here, Janus ScXY (X$\neq$Y=Cl, Br and I) monolayers are predicted to be in-plane piezoelectric ferromagnetic (FM) semiconductors with dynamical, mechanical and thermal stabilities. The predicted piezoelectric strain coefficients $d_{11}$ and $d_{31}$ (absolute values) are higher than ones of most 2D materials. Moreover, the $d_{31}$ (absolute value) of ScClI reaches up to 1.14 pm/V, 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 a 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 (AVHE), and the hole carriers of $\Gamma$ valley move in a straight line. These findings could pave the way for designing piezoelectric and valleytronic devices., Comment: 7 pages,7 figures

Two-dimensional ($2$D) semi-Dirac systems, such as $2$D black phosphorus and arsenene, can exhibit a rich topological phase transition between insulating, semi-Dirac, and band inversion phases when subjected to an external modulation. How these phase transitions manifest within the quantum transport and shot noise signatures remain an open question thus far. Here, we show that the Fano factor converges to the universal $F\approx0.179$ at the semi-Dirac phase, and transits between the sub-Poissonian ($F\approx1/3$) and the Poissonian shot noise ($F\approx1$) limit at the band inversion and the insulating phase, respectively. Furthermore, the conductance of $2$D semi-Dirac system converges to the contrasting limit of $G/G_0 \rightarrow 1/d$ and $G/G_0 \rightarrow0$ at the band inversion and the insulating phases, respectively. The quantum tunneling spectra exhibits a peculiar coexistence of massless and massive Dirac quasiparticles in the band inversion regime, thus providing a versatile sandbox to study the tunneling behavior of various Dirac quasiparticles. These findings reveal the rich interplay between band topology and quantum transport signatures, which may serve as smoking gun signatures for the experimental studies of semi-Dirac systems near topological phase transition., Comment: Submitted to APL special issue, review in progress

Recent experiment has uncovered semimetal bismuth (Bi) as an excellent electrical contact to monolayer MoS$_2$ with ultralow contact resistance. The contact physics of the broader semimetal/monolayer-semiconductor family beyond Bi/MoS$_2$, however, remains largely unexplored thus far. Here we perform a comprehensive first-principle density functional theory investigation on the electrical contact properties between six archetypal two-dimensional (2D) transition metal dichalcogenide (TMDC) semiconductors, i.e. MoS$_2$, WS$_2$, MoSe$_2$, WSe$_2$, MoTe$_2$ and WTe$_2$, and two representative types of semimetals, Bi and antimony (Sb). As Bi and Sb work functions energetically aligns well with the TMDC conduction band edge, Ohmic or nearly-Ohmic $n$-type contacts are prevalent. The interlayer distance of semimetal/TMDC contacts are significantly larger than that of the metal/TMDC counterparts, which results in only weak metalization of TMDC upon contact formation. Intriguingly, such weak metalization generates semimetal-induced gap states (MIGS) that extends below the conduction band minimum, thus offering an effective mechanism to reduce or eliminate the $n$-type Schottky barrier height (SBH) while still preserving the electronic structures of 2D TMDC. A modified Schottky-Mott rule that takes into account SMIGS, interface dipole potential, and Fermi level shifting is proposed, which provides an improved agreement with the DFT-simulated SBH. We further show that the tunneling-specific resistivity of Sb/TMDC contacts are generally lower than the Bi counterparts, thus indicating a better charge injection efficiency can be achieved through Sb contacts. Our findings reveal the promising potential of Bi and Sb as excellent companion electrode materials for advancing 2D semiconductor device technology., Comment: 12 pages, 7 figures

Recent breakthroughs in Josephson diodes dangle the possibility of extending conventional non-reciprocal electronics into the realm of superconductivity. While a strong magnetic field is recognized for enhancing diode efficiency, it concurrently poses a risk of undermining the essential superconductivity required for non-dissipative devices. To circumvent the need for magnetic-based tuning, we propose a field-effect Josephson diode based on the electrostatic gate control of finite momentum Cooper pairs in asymmetric spin-momentum-locking states. We propose two possible implementations of our gate-controlled mechanism: (i) a topological field-effect Josephson diode in time-reversal-broken quantum spin Hall insulators; and (ii) semiconductor-based field-effect Josephson diodes attainable in current experimental setups involving a Zeeman field and spin-orbit coupling. Notably, the diode efficiency is highly enhanced in the topological field-effect Josephson diode because the current carried by the asymmetric helical edge states is topologically protected and can be tuned by local gates. In the proposed Josephson diode, the combination of gates and asymmetric spin-momentum-locking nature is equivalent to that of a magnetic field, thus providing an alternative electrical operation in designing nonreciprocal superconducting devices., Comment: 24 pages, 14 figures

Realizing both ultra-low breakdown voltage and ultra-high gain has been one of the major challenges in the development of high-performance avalanche photodetector. Here, we report that an ultra-high avalanche gain of 3*10^5 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 1.5E_g/e with E_g the band gap of semiconductor. We develop a two-dimensional impact ionization model and uncover that observation of high gain at low breakdown voltage arises from reduced dimensionality of electron-phonon (e-ph) scattering in the layered InSe flake. Our findings open up a promising avenue for developing novel weak-light detectors with low energy consumption and high sensitivity.

Valleytronic materials can provide new degrees of freedom to future electronic devices. In this work, the concepts of the ferrovalley metal (FVM) and valley gapless semiconductor (VGS) are proposed, which can be achieved in valleytronic bilayer systems by electric-field tuning, where the interaction between out-of-plane ferroelectricity and A-type antiferromagnetism can induce layer-polarized anomalous valley Hall (LP-AVH) effect. The K and -K valleys of FVM are both metallic, and electron and hole carriers simultaneously exist. In the extreme case, the FVM can become VGS by analogizing spin gapless semiconductor (SGS). Moreover, it is proposed that the valley splitting enhancement and valley polarization reversal can be achieved by electric field in valleytronic bilayer systems. Taking the bilayer $\mathrm{RuBr_2}$ as an example, our proposal is confirmed by the first-principle calculations. The FVM and VGS can be achieved in bilayer $\mathrm{RuBr_2}$ by applying electric field. With appropriate electric field range, increasing electric field can enhance valley splitting, and the valley polarization can be reversed by flipping electric field direction. To effectively tune valley properties by electric field in bilayer systems, the parent monolayer should possess out-of-plane magnetization, and have large valley splitting. Our results shed light on the possible role of electric field in tuning valleytronic bilayer systems, and provide a way to design the ferrovalley-related material by electric field., Comment: 7 pages, 7 figures

Two-dimensional (2D) niobium oxydihalide NbOI$_2$ has been recently demonstrated as an excellent in-plane piezoelectric and nonlinear optical materials. Here we show that Janus niobium oxydihalide, NbO$XY$ (X, Y = Cl, Br, I and X$\neq$Y), is a multifunctional anisotropic semiconductor family with exceptional piezoelectric, electronic, photocatalytic and optical properties. NbO$XY$ are stable and mechancially flexible monolayers with band gap around the visible light regime of $\sim 1.9$ eV. The anisotropic carrier mobility of NbO$XY$ lies in the range of $10^3 \sim 10^4$ cm$^2$V$^{-1}$s$^{-1}$, which represents some of the highest among 2D semiconductors of bandgap $\gtrsim 2$ eV. Inversion symmetry breaking in Janus NbO$XY$ generates sizable out-of-plane $d_{31}$ piezoelectric response while still retaining a strong in-plane piezoelectricity. Remarkably, NbO$XY$ exhibits an additional out-of-plane piezoelectric response, $d_{32}$ as large as 0.55 pm/V. G$_0$W$_0$-BSE calculation further reveals the strong linear optical dichroism of NbO$XY$ in the visible-to-ultraviolet regime. The optical absorption peaks with $14\sim18$ \% in the deep UV regime ($5\sim6$ eV), outperforming the vast majority of other 2D materials. The high carrier mobility, strong optical absorption, sizable built-in electric field and band alignment compatible with overall water splitting further suggest the strengths of NbO$XY$ in energy conversion application. We further propose a directional stress sensing device to demonstrate how the out-of-plane piezoelectricity can be harnessed for functional device applications. Our findings unveil NbO$XY$ as an exceptional multifunctional 2D semiconductor for flexible electronics, optoelectronics, UV photonics, piezoelectric and sustainable energy applications., Comment: 16 Pages, 7 Figures, 3 Tables

Two-dimensional (2D) layered dielectrics offers a compelling route towards the design of next-generation ultimately compact nanoelectronics. Motivated by recent high-throughput computational prediction of LaO$X$ ($X$ = Br, Cl) as an exceptional 2D dielectrics that significantly outperforms HfO$_2$ even in the monolyaer limit, we investigate the interface properties between LaOX and the archetypal 2D semiconductors of monolayer transition metal dichacolgenides (TMDCs) $M$S$_2$ ($M$ = Mo, W) using first-principle density functional theory simulations. We show that LaO$X$ monolayers interacts weakly with $M$S$_2$ via van der Waals forces with negligible hybridization and interfacial charge transfer, thus conveniently preserving the electronic properties of 2D TMDCs upon contact formation. The conduction and valance band offsets of the interfaces exhibit a sizable value ranging from 0.7 to 1.4 eV, suggesting the capability of LaO$X$ as a gate dielectric materials. Based on Murphy-Good electron emission model, we demonstrate that LaOCl/MoS$_2$ is a versatile dielectric/semiconductor combinations that are compatible to both NMOS and PMOS applications with leakage current lower than $10^{-7}$ Acm$^{-2}$, while LaO$X$/WS$_2$ is generally compatible with PMOS application. The presence of an interfacial tunneling potential barrier at the van der Waals gap further provide an additional mechanism to suppress the leakage current. Our findings reveal the role LaO$X$ as an excellent dielectric companion to 2D TMDC and shall provide useful insights for leveraging the dielectric strength of LaO$X$ in the design of high-performance 2D nanodevices., Comment: 10 pages, 4 Figures, 3 Tables

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 (EOT), excellent gate control, and low leakage currents. Here, we report liquid metal printed ultrathin and scalable Ga2O3 dielectric for 2D electronics and electro-optical devices. We directly visualize the atomically smooth Ga2O3/WS2 interfaces enabled by the conformal nature of liquid metal printing. We demonstrate atomic layer deposition compatibility with high-k Ga2O3/HfO2 top-gate dielectric stacks on chemical vapour deposition grown monolayer WS2, achieving EOTs of ~1 nm and subthreshold swings down to 84.9 mV/dec. Gate leakage currents are well within requirements for ultra-scaled low-power logic circuits. Our results show that liquid metal printed oxides can bridge a crucial gap in scalable dielectric integration of 2D materials for next-generation nano-electronics.

The manipulation of the Rashba spin-splitting is crucial for the development of nanospintronic technology. Here, it is proposed that the Rashba spin-splitting can be turned on and off by reversing electric-field direction. By the first-principle calculations, our proposal is illustrated by a concrete example of Janus monolayer RbKNaBi. The designed RbKNaBi possesses dynamical, thermal and mechanical stability, and is a large-gap quantum spin Hall insulator (QSHI) with Rashba spin-splitting near the Fermi level. A small built-in electric field is predicted due to very small electronegativity difference between the bottom and top atoms, which is very key to switch Rashba spin-splitting through the experimentally available electric field intensity. Due to out-of-plane structural asymmetry, the Janus monolayer has distinctive behaviors by applying external electric field $E$ with the same magnitude but different directions ($z$ or $-z$). Our results reveal that the Rashba energy ($E_R$) and Rashba constant ($\alpha_R$) are increased by the positive $E$, while a negative $E$ suppresses the Rashba splitting to disappear, and then appears again. In a certain $E$ region (0.15 $\mathrm{V/\AA}$ to 0.25 $\mathrm{V/\AA}$), switching Rashba spin-splitting can be achieved by only reversing electric-field direction. Besides, the piezoelectric strain coefficients $d_{11}$ and $d_{31}$ (5.52 pm/V and -0.41 pm/V) are predicted, which are higher than or compared with those of many 2D materials. By piezoelectric effect, the strain can also be used to tune Rashba spin-splitting of RbKNaBi. Moreover, a possible spintronic device is proposed to realize the function of spintronic switch., Comment: 9 pages,10 figures

Topological Dirac semimetals (TDSM), such as Cd$_3$As$_2$ and Na$_3$Bi, exhibits strong optical dichroism with contrasting dielectric permittivity along different crystal axes. However, such optical dichroism is often overlooked in the study of TDSM-based optoelectronic devices, and whether such optical dichroism can lead to unique functionalities not found under the isotropic approximation remain an open question thus far. Here we show that the optical dischroism in TDSM lead to starkly different terahertz (THz) responses and device performance as compared to the isotropic case. Using finite-difference time-domain simulations of a Cd$_3$As$_2$-based metasurface, we demonstrate that such optical dichroism can lead to an unexpected THz wave polarization conversion even if the metasurface structure remains C$_4$ four-fold rotationally symmetric, a practically useful feature not achievable under the isotropic model of TDSM. Our findings concretely reveal the contrasting spectral response between isotropic and anisotropic media, and shed important light on the capability of anisotropic TDSM in THz applications, leading not just to the more accurate device modelling, but also a new route in realizing THz waves polarization conversion without the need of complex device morphology commonly employed in conventional polarization converters., Comment: 7 pages, 4 figures

Valleytronics has been widely investigated for providing new degrees of freedom to future information coding and processing. Here, it is proposed that valley polarization can be achieved by electric field induced magnetic anisotropy (MA) transformation. Through the first-principle calculations, our idea is illustrated by a concrete example of $\mathrm{VSi_2P_4}$ monolayer. The increasing electric field can induce a transition of MA from in-plane to out-of-plane by changing magnetic anisotropy energy (MAE) from negative to positive value, which is mainly due to increasing magnetocrystalline anisotropy (MCA) energy. The out-of-plane magnetization is in favour of spontaneous valley polarization in $\mathrm{VSi_2P_4}$. Within considered electric field range, $\mathrm{VSi_2P_4}$ is always ferromagnetic (FM) ground state. In a certain range of electric field, the coexistence of semiconductor and out-of-plane magnetization makes $\mathrm{VSi_2P_4}$ become a true ferrovalley (FV) material. The anomalous valley Hall effect (AVHE) can be observed under in-plane and out-of-plane electrical field in $\mathrm{VSi_2P_4}$. Our works pave the way to design the ferrovalley material by electric field., Comment: 6 pages, 6 figures. arXiv admin note: text overlap with arXiv:2207.13420

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 of $\mathrm{VSi_2P_4}$ by using the generalized gradient approximation plus $U$ (GGA+$U$) approach. For large $U$, 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, monolayer $\mathrm{VSi_2P_4}$ undergoes ferrovalley (FV), half-valley-metal (HVM), valley-polarized quantum anomalous Hall insulator (VQAHI), HVM and FV states with increasing $U$. However, for assumptive in-plane MA, there is no special quantum anomalous Hall (QAH) state and spontaneous valley polarization within considered $U$ range. According to the MAE and electronic structure with fixed out-of-plane or in-plane MA, the intrinsic phase diagram shows common magnetic semiconductor (CMS), FV and VQAHI in monolayer $\mathrm{VSi_2P_4}$. At representative $U$$=$3 eV widely used in references, $\mathrm{VSi_2P_4}$ can be regarded as a 2D-$XY$ magnet, 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 monolayer $\mathrm{VSi_2P_4}$., Comment: 7 pages,7 figures. arXiv admin note: text overlap with arXiv:2205.07012

For two-dimensional (2D) material, piezoelectric ferromagnetism (PFM) with large out-of-plane piezoresponse is highly desirable for multifunctional ultrathin piezoelectric device application. Here, we predict that Janus monolayer CrSCl is an out-of-plane ferromagnetic (FM) semiconductor with large vertical piezoelectric response and high Curie temperature. The predicted out-of-plane piezoelectric strain coefficient $d_{31}$ is -1.58 pm/V, which is higher than ones of most 2D materials (compare absolute values of $d_{31}$). The large out-of-plane piezoelectricity is robust against electronic correlation and biaxial strain, confirming reliability of large $d_{31}$. Calculated results show that tensile strain is conducive to high Curie temperature, large magnetic anisotropy energy (MAE) and large $d_{31}$. Finally, by comparing $d_{31}$ of CrYX (Y=S; X=Cl, Br I) and CrYX (Y=O; X=F, Cl, Br), we conclude that the size of $d_{31}$ is positively related to electronegativity difference of X and Y atoms. Such findings can provide valuable guidelines for designing 2D piezoelectric materials with large vertical piezoelectric response., Comment: 6 pages, 5 figures

Two-dimensional (2D) materials van der Waals heterostructures (vdWHs) provides a revolutionary route towards high-performance solar energy conversion devices beyond the conventional silicon-based pn junction solar cells. Despite tremendous research progress accomplished in recent years, the searches of vdWHs with exceptional excitonic solar cell conversion efficiency and optical properties remain an open theoretical and experimental quest. Here we show that the vdWH family composed of MoSi$_2$N$_4$ and WSi$_2$N$_4$ monolayers provides a compelling material platform for developing high-performance ultrathin excitonic solar cells and photonics devices. Using first-principle calculations, we construct and classify 51 types of MoSi$_2$N$_4$ and WSi$_2$N$_4$-based [(Mo,W)Si$_2$N$_4$] vdWHs composed of various metallic, semimetallic, semiconducting, insulating and topological 2D materials. Intriguingly, MoSi$_2$N$_4$/(InSe, WSe$_2$) are identified as Type-II vdWHs with exceptional excitonic solar cell power conversion efficiency reaching well over 20%, which are competitive to state-of-art silicon solar cells. The (Mo,W)Si$_2$N$_4$ vdWH family exhibits strong optical absorption in both the visible and ultraviolet regimes. Exceedingly large peak ultraviolet absorptions over 40%, approaching the maximum absorption limit of a free-standing 2D material, can be achieved in (Mo,W)Si$_2$N$_4$/$\alpha_2$-(Mo,W)Ge$_2$P$_4$ vdWHs. Our findings unravel the enormous potential of (Mo,W)Si$_2$N$_4$ vdWHs in designing ultimately compact excitonic solar cell device technology., Comment: 30 pages, 7 figures

Strain is an effective method to tune the electronic properties of two-dimension (2D) materials, and can induce novel phase transition. Recently, 2D $\mathrm{MA_2Z_4}$ family materials are of interest because of their emerging topological, magnetic and superconducting properties. Here, we investigate the impact of strain effects ($a/a_0$:0.96$\sim$1.04) on the physical properties of Janus monolayer $\mathrm{VSiGeN_4}$ as a derivative of $\mathrm{VSi_2N_4}$ or $\mathrm{VGe_2N_4}$, which possesses dynamical, mechanical and thermal stabilities. For out-of-plane magnetic anisotropy, with increasing strain, $\mathrm{VSiGeN_4}$ undergoes transition between ferrovalley semiconductor (FVS), half-valley-metal (HVM), valley-polarized quantum anomalous Hall insulator (VQAHI), HVM and FVS. These imply twice topological phase transitions, which are related with sign-reversible Berry curvature and band inversion between $d_{xy}$+$d_{x^2-y^2}$ and $d_{z^2}$ orbitals for K or -K valley. The band inversion also leads to transformation of valley splitting strength between valence and conduction bands. However, for in-plane magnetic anisotropy, no special quantum anomalous Hall (QAH) states and valley polarization exist within the considered strain range. The actual magnetic anisotropy energy (MAE) shows no special QAH and HVM states in monolayer $\mathrm{VSiGeN_4}$. Fortunately, these can be easily achieved by external magnetic field, which adjusts the easy magnetization axis of $\mathrm{VSiGeN_4}$ from in-plane one to out-of-plane one. Our findings shed light on how strain can be employed to engineer the electronic states of $\mathrm{VSiGeN_4}$, which may open new perspectives for multifunctional quantum devices in valleytronics and spintronics., Comment: 9 pages, 9 figures

The combination of piezoelectricity and ferromagnetic (FM) order in a two-dimensional (2D) material, namely 2D piezoelectric ferromagnetism (PFM), may open up unprecedented opportunities for novel device applications. Here, we predict an in-plane FM semiconductor Janus monolayer NiClI with considerably large magnetic anisotropy energy (MAE) of 1.439 meV, exhibiting dynamic, mechanical and thermal stabilities. The NiClI monolayer possesses larger in-plane piezoelectricity ($d_{11}$$=$5.21 pm/V) comparable to that of $\mathrm{MoS_2}$. Furthermore, NiClI has huge out-of-plane piezoelectricity ($d_{31}$$=$1.89 pm/V), which is highly desirable for ultrathin piezoelectric device application. It is proved that huge out-of-plane piezoelectricity is robust against electronic correlation, which confirms reliability of huge $d_{31}$. Finally, being analogous to NiClI, PFM with large out-of-plane piezoelectricity can also be achieved in the Janus monolayers of NiClBr and NiBrI, with the predicted $d_{31}$ of 0.73 pm/V and 1.15 pm/V, respectively. The predicted huge out-of-plane piezoelectric response makes Janus monolayer NiClI a good platform for multifunctional semiconductor spintronic applications, which is also compatible with the bottom/top gate technologies of conventional semiconductor nanoelectronic devices., Comment: 6 pages, 4 figures

Multiferroic van der Waals (vdW) heterostrucutres offers an exciting route towards novel nanoelectronics and spintronics device technology. Here we investigate the electronic and transport properties of multiferroic vdW heterostructure composed of ferromagnetic FeCl$_2$ monolayer and ferroelectric Sc$_2$CO$_2$ monolayer using first-principles density functional theory and quantum transport simulations. We show that FeCl$_2$/Sc$_2$CO$_2$ heterostructure can be reversibly switched from semiconducting to half-metallic behavior by electrically modulating the ferroelectric polarization states of Sc$_2$CO$_2$. Intriguingly, the half-metallic phase exhibits a Type-III broken gap band alignment, which can be beneficial for tunnelling field-effect transistor application. We perform a quantum transport simulation, based on a \emph{proof-of-concept} two-terminal nanodevice, to demonstrate all-electric-controlled valving effects uniquely enabled by the nonvolatile ferroelectric switching of the heterostructure. These findings unravels the potential of FeCl$_2$/Sc$_2$CO$_2$ vdW heterostructures as a building block for designing a next generation of ultimately compact information processing, data storage and spintronics devices., Comment: 9 pages, 5 figures, accepted for publication in Physical Review B (2022)