Van Der Waals Heterostructures Research Articles

Organic-Inorganic Rubrene/WS2 Heterostructure for Broadband Detection and Polarization Imaging.

Organic single crystals exhibit improved carrier mobility, longer exciton diffusion length, anisotropic charge transport, and unique linear dichroism, while its high exciton binding energy seriously limits the free-carrier generation and photoelectric conversion efficiency. Layered van der Waals heterostructures, which integrate organic crystals with high mobility two-dimensional (2D) inorganic semiconductors, are promising for promoting exciton dissociation and boosting sensitivity by utilizing the interfacial potential and photogating effect. In this work, organic single-crystal rubrene is integrated with a few-layer WS2 to design the high-performance photodetector. The device exhibits an excellent responsivity of 1000 A W-1, and a fast speed of 180 μs, which is far superior to the individual WS2 device. Equally importantly, this device provides excellent polarization detection performance by virtue of the anisotropic properties of rubrene, and the dichroic ratios are 1.56, 1.5, and 1.7 for 375, 405, and 658 nm irradiation, respectively. Finally, several high-resolution single-pixel broadband polarization imaging was demonstrated. Our work shows that organic-inorganic heterostructure is an essential candidate for improving optoelectronics performance and has potential for polarization imaging.

Thermodynamics and electronic structure of edges in monolayer MoSi2N4

MoSi2N4 is a two-dimensional ternary nitride semiconductor that has attracted attention for its excellent mechanical and thermal properties. Theoretical studies predict that zigzag edges of this material can host magnetic edge states and Dirac fermions, but the stability of such edges has not been examined. Here, we present a density functional theory study of the electronic and thermodynamic properties of MoSi2N4 edges. We develop a (partial) ternary phase diagram that identifies a region of chemical potentials within which MoSi2N4 is stable over competing elemental or binary phases. Based on this phase diagram, we determine the thermodynamic stability of several armchair and zigzag edges and elucidate their electronic structures. Bare zigzag edges, predicted to host exotic electronic states, are found to be substantially higher in energy than armchair edges and, thus, unlikely to occur in practice. However, with hydrogen passivation, these zigzag edges can be stabilized relative to their armchair counterparts while retaining metallicity and magnetic order. Our analysis provides a solid thermodynamic basis for further exploration of MoSi2N4 in nanoscale electronics and spintronics.

Superlubric Sliding of Graphene Auto-Kirigami with Interfaces Containing Self-Assembled Stripe-Pattern Adsorbates.

Van der Waals heterostructures formed by stacked 2D materials show exceptional electronic, mechanical, and optical properties. Superlubricity, a condition where atomically flat, incommensurate planes of atoms result in ultra-low friction, is a prime example enabling, for example, self-assembly of optically visible graphene nanostructures in air via a sliding auto-kirigami process. Here, it is demonstrated that a subtle but ubiquitous adsorbate stripe structure found on graphene and graphitic surfaces in ambient conditions remains stable within the interface between twisted graphene layers as they slide over each other. Despite this contamination, the interface retains an exceptional superlubricious state with an estimated upper bound frictional shear strength of 10kPa, indicating that direct atomic incommensurate contact is not required to achieve ambient superlubricity for 2D materials. The results suggest that any phenomena depending on 2D heterostructure interfaces such as exotic electronic behavior may need to consider the presence of stripe adsorbate structures that remain intercalated.

Ultrafast Phase-Control of the Nonlinear Optical Response of 2D Semiconductors

Ultrafast Phase-Control of the Nonlinear Optical Response of 2D Semiconductors

Symmetry-breaking-enhanced power conversion efficiency of 2D van der Waals heterostructures

Symmetry-breaking plays a crucial role in determining the property and functionality of materials. Here, we demonstrate that symmetry-breaking can dramatically enhance the power conversion efficiency (PCE) of a two-dimensional (2D) van der Waals (vdW) heterostructure solar cell by taking a γ-phosphorus-carbide (PC)-based vdW heterostructure as a model. Thanks to its four-atom-layer structure of γ-PC, both alternately arranging P and C atoms to form a Janus structure and sliding C atom layer to change space group are two effective methods to break the symmetry. We find that in comparison with a symmetric configuration, the PCE of γ-PC/MoS2N4 with symmetry-breaking could be increased by 257.2% and 270% via forming a Janus structure and the change in space group, respectively. Particularly, the PCE of symmetry-broken γ-PC/MoSi2N4 can be further increased to 21.35% under an appropriate tensile strain, which could be attributed to small conduction band offset between constituent monolayers and suitable donor bandgap. Our study showcases that tuning the symmetry of multi-atom-layer 2D materials is an effective strategy to realize enhancement of the performance for 2D materials-based optoelectronic devices.

Fast and high-responsivity MoS2/MoSe2 heterostructure photodetectors enabled by van der Waals contact interfaces

Two-dimensional (2D) materials are ideal candidates for building optoelectronic devices, owing to their fascinating photoelectric properties. However, most photodetectors based on individual 2D materials face difficulties in achieving both high responsivity and fast response. In this paper, we have fabricated high-quality vertically stacked MoS2/MoSe2 van der Waals (vdW) heterostructures using dry transfer method. The strong built-in electric field at the interface of type II heterostructure effectively facilitates the separation of photogenerated carriers. The vdW contact between channel material and transferred metal electrode effectively avoids the introduction of defects. These methods effectively enhance the performance of hybrid devices. Under 532 nm laser illumination, this photodetector exhibits high responsivity (528.1 A/W) and fast photoresponse (rise time ∼3.0 μs/decay time ∼31.3 μs). Furthermore, we demonstrated single-pixel image sensing capabilities of the device at room temperature across various modulation frequencies. Importantly, imaging at a frequency as high as 15 000 Hz was attained, indicating its great potential for next-generation, high-performance single-pixel image sensing applications.

Ultralow-Frequency Tip-Enhanced Raman Scattering Discovers Nanoscale Radial Breathing Mode on Strained 2D Semiconductors.

Collective excitations including plasmons, magnons, and layer-breathing vibration modes emerge at an ultralow frequency (<1 THz) and are crucial for understanding van der Waals materials. Strain at the nanoscale can drastically change the property of van der Waals materials and create localized states like quantum emitters. However, it remains unclear how nanoscale strain changes collective excitations. Herein, ultralow-frequency tip-enhanced Raman spectroscopy (TERS) with sub-10nm resolution under ambient conditions is developed to explore the localized collective excitation on monolayer semiconductors with nanoscale strains. A new vibrational mode is discovered at around 12 cm-1 (0.36 THz) on monolayer MoSe2 nanobubbles and it is identified as the radial breathing mode (RBM) of the curved monolayer. The correlation is determined between the RBM frequency and the strain by simultaneously performing deterministic nanoindentation and TERS measurement on monolayer MoSe2. The generality of the RBM in nanoscale curved monolayer WSe2 and bilayer MoSe2 is demonstrated. Using the RBM frequency, the strain of the monolayer MoSe2 on the nanoscale can be mapped. Such an ultralow-frequency vibration from curved van der Waals materials provides a new approach to study nanoscale strains and points to more localized collective excitations to be discovered at the nanoscale.

A direct Z-scheme GaTe/AsP van der Waals heterostructure: A promising high efficiency photocatalyst for overall water splitting with strong optical absorption and superior catalytic activity

The existing energy crisis and environmental pollution require an innovative approach to hydrogen production. Photocatalytic water-splitting has emerged as a potential solution, but the development of efficient photocatalysts remains the key challenge. Here, we employ first-principles calculations to investigate the structural, electronic, optical and photocatalytic characteristics of a van der Waals heterojunction comprising GaTe and AsP monolayers. The constructed GaTe/AsP heterojunction is thermodynamic, dynamical and thermal stable. The smaller indirect bandgap 1.68 eV than 2.21 eV and 2.45 eV for the constituent GaTe and AsP monolayers respectively, enhances the optical absorption of the GaTe/AsP heterojunction in visible and ultraviolet (UV) regions. The type-II band alignment of the GaTe/AsP heterojunction makes an efficient separation of photogenerated electrons and holes to different layers and extension their lifespans. The built-in electric field from GaTe side to AsP side induces a direct Z-scheme heterojunction photocatalyst with high redox reaction kinetic and high solar-to-hydrogen efficiency of 14.10 %. Our study demonstrates that the GaTe/AsP heterostructure is as efficient photocatalysts for overall water-splitting.

2D Reconfigurable van der Waals Heterojunction for Logic Gate Circuits and Wide-Spectrum Photodetectors via Sulfur Substitution and Band Matching.

The attractive physical properties of two-dimensional (2D) semiconductors in group IVA-VIA have been fully revealed in recent years. Combining them with 2D ambipolar materials to construct van der Waals heterojunctions (vdWHs) can offer tremendous opportunities for designing multifunctional electronic and optoelectronic devices, such as logic switching circuits, half-wave rectifiers, and broad-spectrum photodetectors. Here, an optimized SnSe0.75S0.25 is grown to design a SnSe0.75S0.25/MoTe2 vdWH for logic operation and wide-spectrum photodetection. Benefiting from the excellent gate modulation under the appropriate sulfur substitution and type-II band alignment, the device exhibits reconfigurable antiambipolar and ambipolar transfer behaviors at positive and negative source-drain voltage (Vds), enabling stable XNOR logic operation. It also features a gate-modulated positive and negative rectifying behavior with rectification ratios of 265:1 and 1:196, confirming its potential as half-wave logic rectifiers. Besides, the device can respond from visible to infrared wavelength up to 1400 nm. Under 635 nm illumination, the maximum responsivity of 1.16 A/W and response time of 657/500 μs are achieved at the Vds of -2 V. Furthermore, due to the strong in-plane anisotropic structure of SnSe0.75S0.25-alloyed nanosheet and narrow bandgap of 2H-MoTe2, it shows a broadband polarization-sensitive function with impressive photocurrent anisotropic ratios of 15.6 (635 nm), 7.0 (808 nm), and 3.7 (1310 nm). The direction along the maximum photocurrent can be reconfigurable depending on the wavelengths. These results indicate that our designed alloyed SnSe0.75S0.25/MoTe2 vdWH has reconfigurable logic operation and broadband photodetection capabilities in 2D multifunctional integrated circuits.

Large-Scale Direct Growth of Monolayer MoS2 on Patterned Graphene for van der Waals Ultrafast Photoactive Circuits.

Two-dimensional (2D) van der Waals heterostructures combine the distinct properties of individual 2D materials, resulting in metamaterials, ideal for emergent electronic, optoelectronic, and spintronic phenomena. A significant challenge in harnessing these properties for future hybrid circuits is their large-scale realization and integration into graphene interconnects. In this work, we demonstrate the direct growth of molybdenum disulfide (MoS2) crystals on patterned graphene channels. By enhancing control over vapor transport through a confined space chemical vapor deposition growth technique, we achieve the preferential deposition of monolayer MoS2 crystals on monolayer graphene. Atomic resolution scanning transmission electron microscopy reveals the high structural integrity of the heterostructures. Through in-depth spectroscopic characterization, we unveil charge transfer in Graphene/MoS2, with MoS2 introducing p-type doping to graphene, as confirmed by our electrical measurements. Photoconductivity characterization shows that photoactive regions can be locally created in graphene channels covered by MoS2 layers. Time-resolved ultrafast transient absorption (TA) spectroscopy reveals accelerated charge decay kinetics in Graphene/MoS2 heterostructures compared to standalone MoS2 and upconversion for below band gap excitation conditions. Our proof-of-concept results pave the way for the direct growth of van der Waals heterostructure circuits with significant implications for ultrafast photoactive nanoelectronics and optospintronic applications.

Multiferroicity and Topology in Twisted Transition Metal Dichalcogenides.

Van der Waals heterostructures have recently emerged as an exciting platform for investigating the effects of strong electronic correlations, including various forms of magnetic or electrical orders. Here, we perform an unbiased exact diagonalization study of the effects of interactions on topological flat bands of twisted transition metal dichalcogenides (TMDs) at odd integer fillings. For hole-filling ν_{h}=1, we find that the Chern insulator phase, expected from interaction-induced spin-valley polarization of the bare bands, is quite fragile, and gives way to spontaneous multiferroic order-coexisting ferroelectricity and ferromagnetism, in the presence of long-range Coulomb repulsion. We provide a simple real-space picture to understand the phase diagram as a function of interaction range and strength. Our findings establish twisted TMDs as a novel and highly tunable platform for multiferroicity, and we outline a potential route towards electrical control of magnetism in the multiferroic phase.

Controlled Fabrication of Metallic MoO2 Nanosheets towards High-Performance p-Type 2D Transistors.

Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDCs) are extensively employed as channel materials in advanced electronic devices. The electrical contacts between electrodes and 2D semiconductors play a crucial role in the development of high-performance transistors. While numerous strategies for electrode interface engineering have been proposed to enhance the performance of n-type 2D transistors, upgrading p-type ones in a similar manner remains a challenge. In this work, significant improvements in a p-type WSe2 transistor are demonstrated by utilizing metallic MoO2 nanosheets as the electrode contact, which are controllably fabricated through physical vapor deposition and subsequent annealing. The MoO2 nanosheets exhibit an exceptional electrical conductivity of 8.4 × 104 S m‒1 and a breakdown current density of 3.3 × 106 A cm‒2. The work function of MoO2 nanosheets is determined to be ≈5.1eV, making them suitable for contacting p-type 2D semiconductors. Employing MoO2 nanosheets as the electrode contact in WSe2 transistors results in a notable increase in the field-effect mobility to 92.0 cm2 V‒1 s‒1, which is one order of magnitude higher than the counterpart devices with conventional electrodes. This study not only introduces an intriguing 2D metal oxide to improve the electrical contact in p-type 2D transistors, but also offers an effective approach to fabricating all-2D devices.

Room Temperature Emission Line Narrowing and Long‐Range Photon Transport in Colloidal Quantum Wells Coupled to Metasurface Resonance

AbstractHighly efficient and spectrally pure single photon sources are desirable in fundamental studies of quantum physics and in many varied applications like in quantum metrology and quantum cryptography. 2D semiconductor colloidal quantum wells (CQWs) are quite appropriate as nanoscale photon sources because of their giant oscillator strengths and large absorption cross sections. The integration of such sources with dielectric metasurfaces exhibiting narrow resonances provides an excellent platform for highly efficient light‐matter interactions and the development of on‐chip light sources with high spectral purity. Here details on the use of capillary filling method are reported to achieve photonic coupling of CQWs to a metasurface resonator (MSR) featuring a square‐lattice geometry of holes on a slab‐waveguide to achieve strongly enhanced and almost spectrally pure emission of ≈3% of the original out‐of‐plane emission line‐width of the quantum emitters at room temperature. Long‐range exciton‐mediated photon transport facilitated by in‐plane slab waveguide modes is demonstrated and a theoretical basis to explain all the experimental data including that in terms of the MSR‐modified Lamb shifts and Purcell decays is provided. The results demonstrate a new platform with emergent photonic properties and suggest possibility of their use in on‐chip photonic quantum information processing.

Harnessing Persistent Photocurrent in a 2D Semiconductor-Polymer Hybrid Structure: Electron Trapping and Fermi Level Modulation for Optoelectronic Memory.

Recently, 2D semiconductor-based optoelectronic memory has been explored to overcome the limitations of conventional von Neumann architectures by integrating optical sensing and data storage into one device. Persistent photocurrent (PPC), essential for optoelectronic memory, originates from charge carrier trapping according to the Shockley-Read-Hall (SRH) model in 2D semiconductors. The quasi-Fermi level position influences the activation of charge-trapping sites. However, the correlation between quasi-Fermi level modulations and PPC in 2D semiconductors has not been extensively studied. In this study, we demonstrate optoelectronic memory based on a 2D semiconductor-polymer hybrid structure and confirm that the underlying mechanism is charge trapping, as the SRH model explains. Under light illumination, electrons transfer from polyvinylpyrrolidone to p-type tungsten diselenide, resulting in high-level injection and majority carrier-type transitions. The quasi-Fermi level shifts upward with increasing temperature, improving PPC and enabling optoelectronic memory at 433 K. Our findings offer valuable insights into optimizing 2D semiconductor-based optoelectronic memory.

Strain-tuned electronic and valley-related properties in Janus monolayers of SWSiX2 (X = N, P, As)

Abstract Exploring novel two-dimensional (2D) valleytronic materials has an essential impact on the design of spintronic and valleytronic devices. Our first principles calculation results reveal that the Janus SWSiX2 (X = N, P, As) monolayer has excellent dynamical and thermal stability. Owing to strong spin-orbit coupling (SOC), the SWSiX2 monolayer exhibits a valence band spin splitting of up to 0.49 eV, making it promising 2D semiconductor for valleytronic applications. The opposite Berry curvatures and optical selection rules lead to the coexistence of valley and spin Hall effects in the SWSiX2 monolayer. Moreover, the optical transition energies can be remarkably modulated by the in-plane strains. Large tensile (compressive) inplane strains can achieve spin flipping in the SWSiN2 monolayer, and induce both SWSiP2 and SWSiAs2 monolayers transit from semiconductor to metal. Our research provides new 2D semiconductor candidates for designing high-performance valleytronic devices.

Unraveling interfacial thermal transport in β-Ga2O3/h-BN van der Waals heterostructures

As global power consumption rapidly increases with generation of significant amount of heat, efficient thermal management in electronic equipments becomes an urgent task, which requires a comprehensive understanding on thermal transport in heterostructures within devices. Here, we present detailed examination on the interfacial thermal transport of van der Waals (vdW) heterostructures, composed of β-Ga2O3 and hexagonal boron nitride (h-BN) multilayers. Through extensive molecular dynamics simulations, we show that the interfacial thermal conductance (ITC) of β-Ga2O3/h-BN system becomes as high as 136.8MWm−2K−1, and the high ITC value results from substantial phonon interaction across the interface. In addition to the pristine interface, the effect of structural modulation including strain, vacancies and substitutional defects in h-BN multilayers on the ITC is also analyzed, and it is demonstrated that there exists ranges of strain values and defect concentrations which increase the ITC, and that the enhanced ITC is the result of the interplay among the interfacial distance, the overlap in the phonon density of states and elastic mismatch between β-Ga2O3 and h-BN multilayers. These results not only provide insights into understanding interfacial phonon transport in vdW systems but also offer guiding principles for designing efficient heat dissipators in device applications.

Density-functional theory study of SnSe/GeSe heterostructure for gaseous sulfur hexafluoride decomposition products sensing

Partial discharge, local overheating and other factors will lead to the decomposition of superior dielectric gas sulfur hexafluoride (SF6) used in gas insulated substations (GIS). Detecting gaseous sulfur hexafluoride (SF6) decomposition products by gas sensors to diagnose early latent insulation failures is a potential approach to guarantee safety and reliability of gas insulated substations (GIS). However, the main difficulties in the detection of SF6 decomposition products lie in sensitivity, operating temperature and sulfur poisoning of the sensor. Metal oxide selenides (MOSs)-based gas sensors suffer from high working temperature, long recovery time, and sulfur poisoning. Two dimensional selenides-based chemiresistor-type gas sensors have been reported to detect certain gases at room temperature. Compared with pristine materials, heterostructures usually have narrower band gaps and higher carrier mobility which promise low power and sensitivity. In this work, a SnSe/GeSe van der Waals heterostructure model is constructed and optimized to investigate the gas sensing properties by density functional theory (DFT) calculations. Compared with the pristine SnSe and the pristine GeSe, the SnSe/GeSe heterostructure exhibits huge adsorption energy and comparatively large charge transfer to the SF6 decomposition gases. The band structure analysis, charge analysis, electron localization function (ELF), and density of states (DOS) analysis suggest that the excellent sensing properties are contributed to the synergistic effect between the SnSe and the GeSe layers: both the layers transfer charge and orbitally interact with gas molecules. Besides, physical adsorption of the SF6 decomposition gases on SnSe/GeSe heterostructure avoids sulfur poisoning of the material, promising the recoverability and repeatability of detection. This study provides theoretical bases for the repeatable detection of SF6 decomposition products by SnSe/GeSe heterostructures and its potential in the design of electronic nose.

Structural, electronic and optical properties of anisotropic AlN/BP van der Waals heterostructures with high carrier mobility and remarkable optical absorption

The structural, electronic and optical properties of van der Waals heterostructures (vdWHs) of AlN/BP 2D layers have been investigated. Using density functional theory (DFT) calculations, six distinct vertical arrangements of insulating plates composed of aluminum nitride (AlN) and boron phosphide (BP) examined. All six AlN/BP-XX (XX = AA, BB, CC, DD, EE, FF) heterostructures exhibit direct bandgap behavior with type-I band alignment. These heterostructures exhibit remarkable optical absorption in the visible and near-infrared regions, and at room temperature, charge carriers exhibit relatively high mobility for holes in one direction and for electrons in the perpendicular direction.All these six AlN/BP vdWHs have high carrier mobility (of the order of 105cm2V-1s-1), which is comparable to materials with high carrier mobility such as graphene. The energy gap of the AlN and BP monolayers are 4.04 eV and 1.4 eV, respectively, by HSE06 approximation, and for AlN/BP heterostructures are about 1.428 eV to 1.550 eV for all cases. The CBO and VBO of the AlN/BP vdWHs heterostructures are 2.21157 eV and 0.2057 eV, respectively.

Electronic Performance and Schottky Contact of 2D GeH/InSe and GeH/In2Se3 Heterostructures: Strain Engineering and Electric Field Tunability

AbstractRecent exciting developments in synthesis and properties study of the germanane (GeH) mono‐layer have inspired us to investigate the structural and electronic properties of the van der Waals heterostructures (HTS) of GeH/InSe and GeH/In2Se3 through a first‐principles methodology. In this study, structural and electronic properties of the HTS are examined thoroughly. GeH/InSe and GeH/In2Se3 are determined as n‐type Schottky with a Schottky barrier height (SBH) of 0.40 eV and n‐type ohmic, respectively. GeH/InSe turns out as a semiconductor with a direct bandgap of 0.62 eV, while GeH/In2Se3 is seen to be a metal. The results show that changing of the bandgap and SBH in very small values. For GeH/In2Se3 the effects are even less substantial, as the metallic or n‐type nature of the material does not change. The biaxial strain and electric field have more tangible effects on the characteristics of the HTS. A mixture of compressive and tensile strain is seen to have the capability of changing GeH/InSe into a metal and at the same time transform it to an n‐type/p‐type ohmic or p‐type Schottky contact. The results given here can guide future research in the field of HTS and especially GeH‐based devices.

Theory of Moiré Magnetism and Multidomain Spin Textures in Twisted Mott Insulator-Semimetal Heterobilayers.

Motivated by the recent experimental developments in van der Waals heterostructures, we investigate the emergent magnetism in Mott insulator-semimetal moiré superlattices by deriving effective spin models and exploring their phase diagram by Monte Carlo simulations. Our analysis indicates that the stacking-dependent interlayer Kondo interaction can give rise to different types of magnetic order, forming domains within the moiré unit cell. In particular, we find that the AB (AA) stacking regions tend to order (anti)ferromagnetically for an extended range of parameters. The remaining parts of the moiré unit cell form ferromagnetic chains that are coupled antiferromagnetically. We show that the decay length of the Kondo interaction can control the extent of these phases. Our results highlight the importance of stacking-dependent interlayer exchange and the rich magnetic spin textures that can be obtained in van der Waals heterostructures.